The entire sequence in "Chuck Versus the Truth" with the Truth Serum which will slowly kill them, right after they get a single dose of the antidote.
Casey: You're a good person Chuck, and I respect that, but I've got a job to do now take that before I shove it down your throat! Chuck: Okay. Okay, fine. Fine. I'll do it. Sarah: Thank you. Chuck: I'll pretend to agree to take it and then I'll run like hell to my sister's room and make her take it! Why did I just say that out loud? Sarah: It's the poison. It makes you tell the truth. Casey: You do that and I'll give chase, put a gun to your head and threaten to pull the trigger if you don't. Chuck: Would you really shoot me?
It only gets better as the episode goes on.
Chuck: Eugh! Not Pretty! Ugly...
Let's not forget:
Chuck: Casey, your jaw was chiseled by Michelangelo himself.
And when Ellie has been poisoned:
Sarah: Ellie, are you okay? Have you done anything unusual today? Ellie: (beat) ...Words taste like peaches.
Not to mention much of the sequence where they were infected with the serum was set to 'Toxic' by Britney Spears.
Casey going undercover at SarahJenny's High School Reunion as the DJ, and dancing to MMMBop by Hanson.
Sarah tells Chuck she has personal plans for the evening in "Chuck Versus the DeLorean." Chuck follows her to find out what's going on. Sarah reveals that she has set up a program designed specifically to sound an alarm on her phone if Chuck decides to stalks her.
Chuck trying to get a message to Casey at Thanksgiving dinner:
Chuck: I'm thankful that Bryce Larkin is dead, and not in my bedroom making out with my new girlfriend. Morgan: Wow, Chuck, that was... dark. Awesome: And specific.
When Casey gets bemused looks after he is able to produce a high C on demand:
Casey: Choir boy. [even more baffled looks] What? I wasn't hatched.
Three simple words from "Chuck Versus the Gravitron:" "Unleash the Casey."
Casey in "Chuck Versus the Angel de la Muerte," loopy on anesthesia. He goes from a very gruff, angry, "No! No!" to a giggly, touchy-feely, "Ooooh!" in .02 seconds. And upon awakening, his first words are a smiley, "Heh, hey Chucky..."
In "Chuck Versus Operation Awesome," Chuck discovers exactly how awesome Awesome is not at lying, culminating in:
"I must caution you that allowing your private life to interfere with your professional one can be dangerous... but off the record, it's about damn time." (click)
Shaw's deadpan "Muhaha" in "Chuck Versus the Ring, Part II."
And then Chuck gets to do it back to him.
In "Chuck Versus the Suitcase," Morgan's presentation about how the new Buy More is too efficiently run, in the form of a monologue as he strolls through the Buy More as he attempts to cause chaos, but the CIA agents hired to run the store as a substation keep fixing everything before anything happens, using all sorts of crazy stuntwork and precise timing. It helps when one of the new Buy More employees is The Man Your Man Could Smell Like.
Kid: I don't wanna be an astronaut anymore, Mommy. I wanna work at the Buy More. Greta: First you have to finish school, little man.
Jeff & Lester's first scene in season 4 has several within three minutes.
Lester: We are not the boys you are looking for. Morgan: These are not the boys we are lo-- Hey, cut it out!
Lester protesting that people have been following them for months after they were accused of blowing up the Buy More, and Casey asking how Lester knows that they weren't just driving behind them.
Lester coming to the assumption that they need Jeff & Lester, so starts demanding a pay rise, the company car & over privileges. Casey promptly shoots him with a tranq gun & Lester drops like a rock, before Casey tries tranqing Jeff... And nothing happens, although Jeff remarks "I think my water just broke", leading to the disgusted Casey firing more tranq darts at Jeff, waiting for Jeff to fall over, before firing more tranq darts. When Jeff remains standing, Morgan just puffs on him & he falls over.
The "Aisle of Terror" in the episode of the same name:
To start with, it was designed by JEFF AND LESTER, using the results of a study Jeff was once in, involving things even the most deranged, fearless lunatics are afraid of. It serves as a Chekhov's Gun which gets turned on Robert Englund, of all people. However, while the most deranged, fearless lunatics may be afraid of everything being shown, for your everyday person it's a list of things that may or may not kinda be disturbing.
Bonus points go to the oh-so terrifying baby in a snail costume and Chuck's high-pitched, half-terrified/half-adoring voice during the sequence.
Chuck: Old people! Black licorice! Man feet! OTTERS!
In "Chuck Versus The Fear Of Death," pretty much any scene where Lester and Jeff are stalking Greta, or Greta has to whip out her knife.
In "Chuck Versus the Leftovers," the first time Volkoff discovers Chuck is his right hand woman's son and immediately goes from trying to kill him to wanting to go to Thanksgiving Dinner with him. This just gets better as, a couple of scenes later, Volkoff is playing Charades (and making strange motions, including galloping and dancing), complete with slow motion and "In the Hall of the Mountain King" playing in the background.
How can you not laugh at Volkoff kissing Chuck and Chuck's face?
In "Chuck Versus the Push Mix", Volkoff describing his personal boat, or in his terms, his "floating fortress of fun". It comes equipped with anti-air missiles and an old-fashioned ice cream parlor!
The first time we see Team Bartowski in "Chuck Versus the Seduction Impossible" is a POV shot from baby Clara with everyone standing over her crib making gooey faces. When Clara starts crying, Casey proclaims "I'm outta here" and makes towards the kitchen. There's also his hilarious reaction to mistakenly believing Alex is pregnant, and Chuck, Sarah and Casey desperately realising they need a mission when the rest of the Bartowski family start planning Chuck and Sarah's wedding.
Chuck and Morgan humming and air drumming the Imperial March to get Morgan psyched up before a mission.
Chuck and Morgan kidnap someone and take them to the apartment.
Are we in a bathroom? No! This is Hell!
Chuck kissing Casey to save him from a virus in "Chuck vs. The Ex".
Casey: I served my country with honor. Please... let me die with dignity!
Even the RING had it's moments.
Vincent: We detected a computer signal similar to the one Orion used in Hong Kong. We've traced it to a retail store in Burbank, California. RING Elder: Is it a Buy More? Vincent: Yes. Would you like me to pick something up for you?
Volkoff just has too many of them.
"I-I know that if you use those tweezers on those rather large hairs in your nostrils it would work wonders. I mean, when was the last time a man expressed...interest in you, hmm? Be honest."
"No, no, no no, no! Please, stop! Stop, stop! I'll tell you everything you want. No, don't! My home address is 17 Tally Place. My dog's name is Kipper. And I had my first sexual experience watching Lawrence of Arabia. I'm not proud of it. I...I came from a broken home."
"Oh cool, a tiny weapons standoff!"
Trying to toss a knife to Chuck on board a plane, but ends up accidentally skewering a mook in the back.
(In a deadpan tone) "Oh my God, this guy just exposed himself to a woman on the Super Shuttle".
Jeff and Lester stalk Shaw.
Jeff: Stalkers log. Stalkie is getting in a gray van with another male possibly for a sexual encounter. Both men are physically fit. Should be lively. Lester: Don't make me be afraid to be alone with you.
The pilot had the one where Sarah dressed as a burglar tries to steal Chuck's computer. Morgan throws stuff at her but she keeps deflecting them and hits Chuck.
Riley reading Volkoff's will to Vivian in a faux-British accent.
"In a World filled with awkward Chuck and Sarah moments, comes a moment so awkward".
In "Chuck Versus the Frosted Tips", we have Chuck resorting to pulling down Morgan's pants, to allow Sarah to tranquilize him.
Also in the same episode, Casey & Gertrude's hot 'slap slap kiss' fight, which ends in Casey raising his gun barrel in a haunting way in front of Gertrude's face. While she's in handcuffs.
There's also Sane!Jeff having none of Lester's usual shenanigans and refusing to go along with it.
Big Mike's response to Morgan's complaint that he and Mrs. Grimes are too loud during sex.
You can't expect to move into the forest and then complain that the wildlife make too much noise. It's beautiful and natural, and frequent.
"Chuck vs Tom Sawyer" (funniest episode ever) has a few such as Emmett seeing Chuck and Jeff hanging out
(to his tape recorder) "I have observed the following Buy More violations: Misappropriation of the Home Theater room, consumption of alcohol after hours and lewd use of a musical montage."
Later Chuck had to stash Jeff at his apartment, much to Ellie and Sarah's chagrin.
Chuck: (to Jeff) "Wild night, huh? We drunk, you got smashed, we just watched and it was very awkward."
Chuck persuades Morgan to help.
Chuck: "Who was the president of the high school audio/visual club? Who was a roadie for Mamma Mia! for 4 straight summers? Who owns his own smoking machine?" Morgan: "I do, okay? Jeff is a loser, dude".
"Chuck Versus the Kept Man" provides a good number of them.
Shortly thereafter, Sarah encounters a Primal Scene that...well:
Verbanski: (offscreen) You've been a naughty, naughty colonel.
(a spank, followed by Casey grunting, as Sarah looks queasy and rushes out the door) Chuck: (catching up with Sarah) Sarah, what's wrong? Sarah: Everything. It's all wrong.
All of Verbaski's brazen ways of seducing Casey.
"Chuck Versus Bo", the whole scene of Intersect!Morgan partying. It starts off with him arriving at a cabin and annnouncing to everyone there: "WHO WANTS TO PARTY WITH THE FRICKING INTERSECT!"
Every scene involving the Vail Buy More, as we see that there's a group eerily similar to the Burbank Buy Morons.
Casey, in general, once again brings the laughs, especially with his reaction upon having to go to the Vail Buy More to complete the final mission.
While Jeff and Lester's Big Damn Heroes moment from "Chuck Versus the Bullet Train" is a certifiable Moment of Awesome, it's got it's hilarious moments too. Particularly when we see Jeff and Lester armed to the teeth with weaponry from Casey's Crown Vic, and threatening the baddie, while Canada's national anthem plays in the background.
Casey: Your country needs you! [[[Beat]]] Lester: Canada?
While "Chuck Versus Sarah" is more of a dramatic (and quite frankly, dark) episode, something has to be said about Morgan fooling around with an invisibility cloak that he stumbles upon while the Carmichael team infiltrates the DARPA building to destroy the Intersect once and for all.
As to be expected, the Grand Finale "Chuck Versus the Goodbye" has it's moments.
Captain Awesome covering Clara's eyes the moment he realises Grandma Frost has a gun out.
Devon: Grandma, what did we say about guns around baby Clara? [Frost lowers her gun] Frost: That it's a no-no. I'm sorry!