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To break the ice on the set, De Niro, a two-time Oscar winner, took the rapper and one-time drug dealer to a firing range to shoot handguns.
"We went a couple of times together," Jackson, 33, tells PEOPLE. "He was a much better shot than I thought he would be. I was impressed."
While Jackson – who was shot nine times at close range eight years ago – may have been wowed by De Niro's way with a gun, he wasn't intimidated by the 65-year-old actor, or his equally legendary Righteous Kill costar, Al Pacino.
"I was comfortable, because I was really well-prepared," says Jackson. "I had worked long and hard with an acting coach specifically for that role."
Jackson says his character in the movie, a street-hustler-turned-nightclub-owner, has little in common with the real life gangsters he met growing up in Queens.
"He is taunting the police and they don’t actually do that," says Jackson. "In reality [gangsters] move away from those type of situations, because ultimately you wont win."
Adds Jackson, "In that life you don’t want no association to them period. You want to avoid police totally."
JOSH & FERGIE: ROCKED BY SCANDAL
Did he cheat with a stripper?
Married less than a year, the couple denies an Atlanta woman’s claims that she and Josh had a fling
Note that this week’s cover of PEOPLE may differ regionally
