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The actor will star alongside Law & Order's Jesse L Martin in Sexual Healing, which chronicles the final three years of the Motown star's life.
It will focus on Gaye's (Martin) emigration to Belgium in 1981 and his comeback the following year after being taken under the wing of promoter Freddy Cousaert (Gandolfini).
The singer was shot and killed by his father on the eve of his 45th birthday in 1984, after he moved into the family home suffering from depression and drug addiction.
The film will be directed by Lauren Goodman and produced by Gandolfini's production company Attaboy Films.
Filming is scheduled to begin in April.
Gandolfini attacked a fan at New York's JFK airport earlier this week.
