He plays the younger version in sci-fi sequel Men in Black III, where Will Smith travels back in time to protect his partner from an alien assassin.
Digital Spy sat down with the suited chameleon to find out about his impromptu dinner table audition for director Barry Sonnenfeld and why he steered well clear of Jones on the set.
"I knew Barry a little bit before this because he used to work with the Coen Brothers," Brolin said. "I gave the Coens an award and it was a fairly funny speech, so Barry wanted to get to know me.
Brolin revealed that his co-star Smith already has plans to make a fourth Men in Black.
"Will had an idea the other day at a press conference that I thought was genius," he said. "We haven't talked about a fourth film, it hasn't been mentioned. I know that Will thought up the idea for the third one on the second film ten years ago.
"I don't know if it's going to take 20 years to put this together, but hopefully not because I think it's a great, great, great idea that he has."
> Will Smith's career in pictures: 'Men in Black', 'Independence Day', more