Valerie was born in Ventor, New Jersey, to Louis and Dorothy Bondo Solanas. Her father sexually molested her; sometime in the 1940's her parents divorced, and Valerie moved with her mother to Washington, D.C.. In 1949 Valerie's mother married Red Moran. Rebellious and stubborn, Valerie disobeyed her parents and refused to stay in Catholic high school; in response her grandfather whipped her.

At the age of 15 in 1951, Valerie ended up on her own. She dated a sailor and may have gotten pregnant by him but still managed to graduate from high school in 1954. She was a good student at the University of Maryland at College Park, supporting herself by working in the psycology department's animal laboratory. She did nearly a year of graduate work in psychology at University of Minnesota.

After college, Solanas panhandled and worked as a prostitute to support herself. She traveled around the country and ended up in Greenwich Village in 1966. There she wrote a play Up Your Ass. Early in 1967 Solanas approached Andy Warhol at his studio, the Factory, about producing Up Your Ass, as a play and gave him her copy of the script.

Later, in May 1967, after Warhol had returned from a trip to France and England, Solanas demanded her script back; Warhol informed her he had lost it. Apparently, Warhol had never any intention to produce Up Your Ass as either a play or a movie. Solanas began telephoning insistently, ordering Warhol to give her money for the play.

In July 1967 Warhol paid Solanas twenty-five dollars for performing in I, a Man, a feature-length film he was making with Paul Morrissey. Valerie appeared as herself, a tough lesbian who rejects the advances of a male stud. Solanas also appeared in a nonspeaking role in Bikeboy, another 1967 Warhol film. She wrote a few sex novels and was paid $500 for one.

On June 3, 1968 Solanas shot Warhol three times. Between the first and second shot, both of which missed, Warhol screamed, "No! No! Valarie, don't do it." Her third shot sent a bullet through Warhol's left lung, spleen, stomach, liver, esophagus and right lung.

That evening, Solanas turned herself in to a rookie traffic officer in Time Square; she said, "The police are looking for me and want me." She then took the .32 automatic and a .22 pistol from the pockets of her raincoat, handing them to the cop. As she did so, she stated that she had shot Andy Warhol and in way of explanation offered, "He had too much control of my life."

Solanas was indicted on charges of attempted murder, assault, and illegal possession of a gun. In August, Solanas was declared incompetent and was sent to Ward Island Hospital. After pleading guilty, Valerie Solanas was sentenced to three years in prison for "reckless assault with intent to harm"; the year she spent in a psychiatric ward awaiting trial counted as time served. It has been suggested that Warhol's refusal to testify against Solanas contributed to the short sentence.

Solanas was released on September 1971 from the New York State Prison for Women at Bedford Hills; she was arrested again November 1971 for threatening letters and calls to various people, including Andy Warhol. In 1973 Solanas was in and out of mental institutions; she spent eight months in South Florida State Hospital in 1975.

Broke and alone, Valerie Solanas died of emphysema and pneumonia in a welfare hotel in the Tenderloin district of San Francisco. She was buried in Virginia, near the home of her mother. Valerie is the subject of the 1996 film I Shot Andy Warhol.