"Ask Noah" - Ultron

It's a little comedic but...

"I am a god you dull creature! And I will not be bullied by a-"

"When you look into the eyes of a child you have raised, no mask in the world can hide that." Dreykov

"With you, an Avenger under my control, I can finally come out of the shadows using the only natural resource that the world has too much of. Girls." Dreykov

"You are the first thing, excuse me, person, that I ever wanted that walked away from me."

―Kilgrave

“I speak many languages.”

“How many?”

”All of them.”

"You embarrassed me! You embarrassed me in front of her!" - Kingpin

(Technically still a villain at this point since he only became a good guy after that meeting with Mobius):

Absolutely not! This is fine Asgardian leather!

Thanos

• I know what it's like to lose. To feel so desperately that you're right, yet to fail nonetheless. It's frightening, turns the legs to jelly. But I ask you, to what end? Dread it. Run from it. Destiny arrives all the same. And now, it's here. Or should I say...I AM

Killmonger

• Just bury me in the ocean, with my ancestors that jumped from the ships, because they knew death was better than bondage.

• How is never as important as why, right?

That first Killmonger quote about being buried at sea is so powerful. I remember the first time I saw the movie, I felt like someone had punched me in the gut.

Oh, definitely the bit when Caecilius meets Dr. Strange! The "Mr. Doctor" - "No. Strange." - "Strange? Well, who am I to judge?" Still cracks me up.

Who the hell is Bucky? - Winter Soldier