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Alas, Poor Villain: Not every Shinma is a Jerkass or a Complete Monster. Some of these are little Aiko aka Baku's "controller", manga!Lemures, the Shinma armor, and the Minami family.
Ho Yay: In the TV series, pretty blatant between Larva and Garline, especially from the latter's side: he acts like a spurned lover, mentions Larva's "beauty", takes his hand, caresses his cheek... Considering that Garline is an Expy of Lemures, it's not really a surprise.
Les Yay: In the manga, the difference between how Reiha treats Ranka and Miyu is very... extreme. When Ranka is injured in the process of sheilding Miyu from her wrath, Reiha becomes very courtly and kisses her wounded hand. Ranka's reaction to this is a shudder.
In the TV series there's also the episode Love of the Dolls where the doll maker/artist Kasumi and her maid/assistant Yuki end up pretty explicitly in a relationship together. Oddly enough, it gave the impression that the viewer should view this as a bittersweet ending, even though their previous dysfunctional relationship had turned pretty wholesome after becoming romantic.
Moral Event Horizon: Many Shinma leap over this limit, but some cases are worse than others.
In the anime, Lemures crosses it with gusto. Not only he kidnaps Larva and seals him away, but he uses a very cruel trap to recruit the Shinma armor. He tricks a desperate young widow into giving him her life to bring her husband back, but once she does so and dies, the hubby's soul is bound to an armor in his Big Fancy House, making him his memory-less and Ax CrazyMook.
Then we have Chisato crossing it in the TV series, when she murders Hisae and Yukari as soon as her Shinma powers awaken. She has kind of an excuse in the case of Hisae since there's some degree of More Than Mind Control from Shidon, but in the case of Yukari she does it outta her free will.
By proxy, Shidon crossed it too. Who is he? Well, he's Chekhov's Gunman Shinma that gave her and Miyu the trinkets that kept Miyu from sensing Chisato's growing Shinma energy. Double when he awakens Chisato's powers for the first time... and manipulates her into killing Hisae.
And the Shinma that manipulated Miho via preying on her insecurities and her gorgeous singing voice is not much better either.
There are MANY of those, actually. Aside of Aiko we have Aya, Mari and her sister Rima, Ruri and Mamoru from the manga; Miyahito, Ryoko, and the Shinma armor from the OAV; and Miho from the TV series as well as Yukari and Hisae.