Carroll Baker was born and raised in Johnstown, Pennsylvania, in a Roman Catholic family, the daughter of Edith Gertrude (nee Duffy) and William Watson Baker, a traveling salesman. She is of Polish descent, which has given rise to a rumor that her birth name was Karolina Piekarski. However, this currently cannot be substantiated by known records. Baker's parents separated when she was eight years old, and she moved with her mother and younger sister, Virginia, to Turtle Creek, Pennsylvania.

Baker portrayed a pacifist Quaker schoolteacher in John Ford's Cheyenne Autumn (1964), and received critical acclaim for the role. She then had a supporting role as Saint Veronica in George Stevens' The Greatest Story Ever Told (1965), and portrayed a cynical, alcoholic movie star in The Carpetbaggers (1964), which brought her a second wave of notoriety in spite of the film's lackluster reviews. The New York Times called the film "a sickly sour distillation" of the source novel, but said Baker's performance "brought some color and a sandpaper personality as the sex-loaded widow." The film was the top moneymaker of that year, with domestic box-office receipts of $13,000,000, and marked the beginning of a tumultuous relationship with the film's producer, Joseph E. Levine.  Based on her Carpetbaggers performance, Levine began to develop Baker as a movie sex symbol, and she appeared posing in the December 1964 issue of Playboy. She was subsequently cast by Levine in the title roles of two 1965 potboilers-- Sylvia, as an ex-prostitute and con artist, and as Jean Harlow in Harlow. Baker appeared on the cover of the Saturday Evening Post on their November 2, 1963, issue dressed as Harlow, promoting the film's upcoming production. In 1965, she became an official celebrity spokesperson for Foster Grant sunglasses and appeared in advertisements for the company. Baker likened this era of her career to "being a beauty contest winner [as opposed to] an actress."  Despite much prepublicity, Harlow received a lukewarm response from critics: Variety referred to Baker's portrayal of Harlow as "a fairly reasonable facsimile, although she lacks the electric fire of the original." Relations between Baker and Levine soured; in a 1965 interview, Baker sardonically commented: "I'll say this about Joe Levine: I admire his taste in leading ladies," which led the press to suspect a rift between the actress and producer. Baker sued Levine over her contract with Paramount Pictures in 1966, and was ultimately fired by Paramount and had her paychecks from Harlow frozen amid the contentious legal dispute; this left Baker hundreds of thousands of dollars in debt (however, she was eventually awarded $1 million in compensation).  In an interview with Rex Reed in his book People Are Crazy Here (1974), Baker revealed that she had felt pressure in both her working relationship with Levine, and her domestic life with her husband, the latter of whom she said wanted to maintain an expensive lifestyle: "We'd been very poor when we started out at the Actors Studio in New York," she told Reed. "I was under contract to Joe Levine, who was going around giving me diamonds and behaving like he owned me. I never slept with him or anything, but everyone thought I was his mistress." In the spring of 1966, Baker returned to theatre, performing in a production of Anna Christie at the Huntington Hartford Theater in Los Angeles. The production was directed by Garfein. The production was heralded as the "theatre event of the week" in Los Angeles, though its reception was middling. Cecil Smith of The Los Angeles Times wrote of the production: "The beautiful Miss Baker's vehicle becomes a hearse." The play was also performed at the Tappan Zee Playhouse in Nyack, New York in June 1966.

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