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Nico rose to prominence as a model. After leaving school at the age of thirteen, she started selling lingerie and soon was spotted by fashion insiders. A year later, her mother found her work as a model in Berlin.

While on a modeling assignment in Ibiza, she met the photographer Herbert Tobias, who gave her the name "Nico" after his ex-boyfriend, filmmaker Nico Papatakis.[citation needed] She soon moved to Paris and worked for Vogue, Tempo, Vie Nuove, Mascotte Spettacolo, Camera, Elle, and other fashion magazines in the late 1950s.

She also claimed to have been briefly hired by Coco Chanel. Despite having dropped out of school at an early age, Nico eventually became fluent in English, Italian, Spanish, and French.

After appearing in several television advertisements, Nico obtained a small role in Alberto Lattuada's film La Tempesta (1958), and then appeared in Rudolph Maté's For the First Time with Mario Lanza later that year.

In 1959, she was invited to the set of Federico Fellini's La dolce vita and attracted the attention of the acclaimed director, who gave her a minor role in the film. By this time, she had moved to New York to take acting classes under the guidance of Lee Strasberg.

After splitting her time between New York and Paris, she landed the lead role in Jacques Poitrenaud's Strip-Tease (1963). She recorded the title track, which was produced by Serge Gainsbourg but not released until 2001, when it was included on CD as part of the French compilation Le Cinéma de Serge Gainsbourg.

In 1962 Nico gave birth to her son, Ari Boulogne, who was fathered by French actor Alain Delon. Although the child was raised mostly by Delon's parents, Delon always denied his paternity.

In 1965, Nico met The Rolling Stones' guitarist, Brian Jones, and recorded her first single, "I'm Not Sayin'" for Andrew Loog Oldham's Immediate label.

Actor Ben Carruthers introduced her to Bob Dylan in Paris that summer. It is said that Dylan wrote the song "I'll Keep It With Mine" for her shortly afterwards.

After being introduced by Bob Dylan, she began working with Andy Warhol and Paul Morrissey on their experimental films, including Chelsea Girls, The Closet, Sunset, and Imitation of Christ.

After Warhol became manager of The Velvet Underground, he proposed that the group take on Nico as a singer. The group consented with considerable reluctance, for both personal and musical reasons - John Cale of the group has described Nico as "tone deaf"; despite this, he would go on to play a major role in her solo career. The group, including Nico, became the musical accompanists for Warhol's Exploding Plastic Inevitable, a multimedia performance featuring film, music, lights and dancers.

Nico sang lead vocals on three songs ("Femme Fatale", "All Tomorrow's Parties" and "I'll Be Your Mirror") and backing vocals on another ("Sunday Morning") on the band's debut record, The Velvet Underground and Nico. Released in 1967, the album went on to prove influential to many future genres, including punk rock and New Wave.

Nico had a short-lived romantic relationship with the main singer and songwriter, Lou Reed. Around this period she was also romantically involved with prominent musicians including Cale, Jim Morrison of The Doors, Jackson Browne, Brian Jones, Tim Buckley, Bob Dylan and Iggy Pop.

Shortly after the album's ensuing tour, Exploding Plastic Inevitable, drew to a close in early 1967, Nico and The Velvet Underground parted ways. Both Reed and John Cale played significant parts in various aspects of her solo career. Over the course of the next 20 years, she recorded a series of critically acclaimed albums, working with the likes of Brian Eno and Phil Manzanera. Cale was particularly involved in her music, producing four of her albums as well as arranging and playing various instruments on the recordings.

For her debut album, 1967's Chelsea Girl, Nico recorded songs by, among others, Bob Dylan, Tim Hardin, Jackson Browne and Velvet Underground members Lou Reed, John Cale and Sterling Morrison, co-writing with Reed and Cale one song, "It Was a Pleasure Then", an eight-minute piece with guitar and violin solos.
Chelsea Girl is a traditional chamber-folk album that influenced the style of artists such as Leonard Cohen, with strings and flute arrangements superimposed by its producer. Nico was not satisfied with the finished album and had little say in production matters.

For her LP The Marble Index, released in 1969, Nico herself wrote the lyrics and the bare bones of the music, which mainly consisted of see-sawing harmonium chords. The arrangements were written by John Cale, who fleshed out Nico's songs with an array of folk and classical instruments. Frazier Mohawk produced the album. Nico's harmonium became her signature instrument for the rest of her career. The album combines classical elements with a European folk sound.

Nico released two more solo albums in the 1970s: Desertshore (1970, again produced by John Cale) and The End (1974, co-produced by Cale and Joe Boyd). Cale played most of the instruments on these records. Nico wrote the music, sang, and played the harmonium. The End also featured Brian Eno on the synthesizer, who also performed on the live album June 1, 1974 with Nico, Cale and Kevin Ayers.

On 13 December 1974, Nico was the support act at Tangerine Dream's infamous concert at Reims Cathedral in Reims, France. The promoter had so greatly oversold the capacity of the venue that members of the audience could not move or reach the outside, eventually resulting in some fans urinating inside the cathedral hall. The Roman Catholic Church denounced these actions, ordered the rededication of the cathedral and banned future performances on church property.

Nico returned to New York in late 1979 where her comeback concert at CBGB in early 1980 was glowingly reviewed in the New York Times.

She began playing regularly at the Mudd Club and other venues with Jim Tisdall accompanying her on harp and Gittler electric guitar, and they went on a sold-out tour of twelve cities in the East and Midwest.

Nico recorded her next studio album, Drama of Exile, in 1981.
It was a departure from her earlier work with John Cale and featured a mixture of rock and Middle Eastern arrangements. She recorded her final solo album, Camera Obscura, in 1985, with John Cale back as producer and The Faction (James Young and Graham Dids) an experimental collection that featured Nico's version of the Richard Rodgers/Lorenz Hart song, "My Funny Valentine". A number of Nico's performances towards the end of her life were recorded and released, including 1982's Heroine, 1986's Behind the Iron Curtain and Live In Tokyo, and her final concert, Fata Morgana, recorded on 6 June 1988, edited extracts of which were also released on Hanging Gardens.

Between 1970 and 1979, Nico made about seven films with French director Philippe Garrel. She met Garrel in 1969 and contributed the song "The Falconer" to his film, Le Lit de la Vierge. Soon after, she was living with Garrel and became a central figure in his cinematic and personal circles.

Nico's first acting appearance with Garrel occurred in his 1972 film, La Cicatrice Intérieure. Nico also supplied the music for this film and collaborated closely with the director. She also appeared in the Garrel films Anathor (1972); the silent Jean Seberg biopic, Les Hautes Solitudes, released in 1974; Un ange passe (1975); Le Berceau de cristal (1976), starring Pierre Clementi, Nico and Anita Pallenberg; and Voyage au jardin des morts (1978). His 1991 film J'entends Plus la Guitare is dedicated to Nico.

Nico was a heroin addict for over 15 years. The biographer Richard Witts speculated that the habit was caused by her traumatic experiences of war and of being an illegitimate child.

In the book Songs They Never Play on the Radio, James Young, a member of Nico's band in the 1980s, recalls many examples of Nico's fiendish behaviour due to addiction. But just before her death she had managed to kick the habit and had embarked on a regimen of exercise and healthy eating.

On 18 July 1988, while on holiday with her son in Ibiza, Spain, Nico had a minor heart attack while riding a bicycle and hit her head as she fell. A passing taxi driver found her unconscious and had difficulty getting her admitted to local hospitals. She was incorrectly diagnosed as suffering from heat-exposure and died the next day. X-rays later revealed a severe cerebral hemorrhage as the cause of her death.

Nico was buried in her mother's plot in Grunewald Forest Cemetery in Berlin. A few friends played a tape of "Mütterlein", a song from Desertshore, at her funeral.