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Trinity: "Neo... nobody has ever done anything like this before."

Neo: "That's why it's going to work."
"A strange game. The only winning move is not to play."
Joshua, War Games
"There is a third option. It involves... murder."

Riku: What are you making me choose now?

DiZ: Will you take the road to light — or the road to darkness?

Riku: Neither. I'm taking the middle road.

DiZ: You mean the twilit road to nightfall?

Riku: No... The road to dawn.
Kingdom Hearts: Chain of Memories (technically taking the fourth option)

Dr. Rumack: What was it we had for dinner tonight?

Elaine Dickinson: Well, we had a choice of steak or fish.

Dr. Rumack: Yes, yes, I remember, I had the lasagna.
"Doakes said I had two choices - kill him or let him go. But he neglected to look behind door number three..."
"One day, someone showed me a glass of water that was half full. And he said, "Is it half full or half empty?" So I drank the water. No more problem."
Alexander Jodorowsky

David: "What? There's a third option? Crazy and daring?"

Fatebane: "Daring, definitely daring... possibly fatal..."

David: "So what else is new?"
"My vengeance will be neither swift nor entertaining! I will mete it out over decades, so that you will wonder if the misery in your life is manifest, the machinations of Leonardo Leonardo, or... some third thing. Good day!"
Leonardo Leonardo, Clerks, the animated series

Batman: I've made my choice... none of the above!

D.A.V.E.: How very predictable. I anticipated you would try to create a third, more favourable option.
The Batman, Gotham's Ultimate Criminal Mastermind
"When forced to choose between the universe and the woman you love, choose both and have the courage to back it up"
The Laws of Super Robot Anime
"There's an old Talaxian expression. 'When the road before you splits in two... take the third path.'"

 Umbridge: So are you Team Edward or Team Jacob?

Sorting Hat: Neither. I'm TEAM DUMBLEDORE!

Umbridge:: Dumbledore's not a fictional character.

Dr.Porkchop: You must choose, sheriff Woody. How shall she die!? Shark!? Or death by monkeys!? CHOOSE.

Woody: I Choose... BUZZ LIGHT-YEAR!

Dr.Porkchop: WHAT!? That's not a choice!

Serenity: Okay, Nesbitt! Which came first: the chicken or the egg?

Nesbitt: The rocket-powered fist!

Serenity: But, that wasn't one of the *hits by a rocket-powered fist*

VII. And Grimma said, We have two choices.

VIII. We can run, or we hide.

IX. And they said, Which shall we do?

X. She said, We shall Fight.

From The Book of Nome, Quarries, Chap. 3, v. VII-X
"Well either one or the other is going to happen. There's no weird third thing."
Liz, Thirty Rock
"I'm not going to deal with this now. It's like the classic debate of why measuring the position of an electron changes its momentum and vice-versa. The only correct answer is to get drunk and set fire to things."
"Choosing isn't always right! Sometimes, not choosing is the correct answer! It may be referred to as the "harem" option!"
Red, Hyperdimension Neptunia (optional skit)
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