Grier was discovered by quickie director Roger Corman, who cast her in his women-in-prison pictures The Big Doll House (1971) and The Big Bird Cage (1972). She became a staple of the blaxploitation movies of the early 1970s, playing big, bold, buxom, and essentially interchangeable roles in such films as Coffy (1973), Foxy Brown (1974) and Sheba, Baby (1975).

With the demise of blaxploitation, Grier's career went into hiatus for some years. She worked her way into progressively larger character roles in the 1980s, including notably the stoned prostitute in Fort Apache the Bronx (1981), a witch in Something Wicked this Way Comes (1983), and Steven Seagal's detective partner in Above the Law (1988). She became a regular on the hit television detective series Miami Vice in 1985.

Ms. Grier highlighted a successful television series during the '90s on the network B.E.T.

Grier re-achieved leading lady status in 1997 as the titular stewardess in Quentin Tarantino's Jackie Brown, which many consider her best work so far. Grier is currently appearing in the television series The L Word.

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