Classic shot of Robert De Niro in Goodfellas. In this shot - SPOILERS - De Niro is coming to the conclusion that he's going to have to kill a member of his crew.
I want to talk about his eye focus/direction. Often when we look at things, and especially people, we're not able to look directly at them for long periods of time. When animating, we often make our characters dart their eyes around, not focusing on things for too long to make it feel more real. But look at this example. Though his eyes are looking around, once they focus on something they stay locked. De Niro's character in Goodfellas is a very intense person who commands respect. When he looks at someone, he stares directly at them, no eyes darts looking away. He's commanding respect/daring someone to challenge him. It's like how a predator would look around a room, and that's what he is...a predator. Keep in mind who your character is and how that changes how they look at things in their world.