Cope's musical career began in July 1977, as bass player with a mythical Liverpool punk rock band known as Crucial Three, which also featured Ian McCulloch (later guitarist and singer for Echo and the Bunnymen) and guitarist Pete Wylie, who later formed The Mighty Wah. Although the Crucial Three lasted for little more than six weeks, and disbanded without ever actually playing a note, all three members went on to lead very successful post-punk bands. Cope went on to form other short-lived bands UH? and A Shallow Madness with McCulloch, before finally achieving fame and success as the singer, original bassist and primary songwriter of The Teardrop Explodes.
In 1981, Cope compiled Fire Escape in the Sky: The Godlike Genius of Scott Walker, which was released by Bill Drummond's Zoo Records. This sparked renewed interest in the work of the reclusive singer; though years later Cope commented that Walker's "Pale White Intellectual" outlook on life no longer held any fascination for him.
After The Teardrop Explodes disbanded in late 1982 following the completion of three albums, Cope returned to live close to his hometown of Tamworth, settling in the nearby village of Drayton Bassett with his new American wife Dorian. In 1983 he recorded some tunes for John Peel's show, re-working these highly introspective works for his first solo album, World Shut Your Mouth, released on Mercury Records in March 1984. This record was followed just six months later by Fried, which featured a sleeve with Cope clad only in a turtle shell. The failure of this record caused Polygram to drop Cope, but he signed a deal with Chris Blackwell's Island Records.
Cope's third solo album was the well-received Saint Julian (produced by Ed Stasium) and released the single "World Shut Your Mouth", which became his biggest solo hit, reaching #19 in the UK in 1986, becoming his only Top 20 single there. The follow-up album My Nation Underground spawned only one Top 40 single in "Charlotte Anne", and Cope fell out with Island Records at this time. Cope found modest American success with "Charlotte Anne" reaching the top of the Modern Rock Tracks. He recorded his next album, the low-fi Skellington, in secret during the course of a single weekend, playing in the same studio used for My Nation Underground. Neither his record company nor management had any desire to release Skellington (Zippo, 1989), and Cope refused to record any other material while he feuded with them to try to get his new work released. This became the first of many feuds with record companies. Cope next released a Texas-only album entitled Droolian (Mofoco, 1990), the profits of which were used to aid of one of his heroes Roky Erickson, who was in jail without legal representation.
When Cope's war with Island Records had abated, he released the double album Peggy Suicide (Island, 1991), which was heralded by critics as his best work thus far. The record was recorded during Margaret Thatcher's Poll Tax Riots, in which Cope took a prominent role, wearing a huge theatrical costume throughout the march. Cope was later featured on the BBC's Poll Tax documentary, a lone protester walking down Whitehall in the costume surrounded by seven lines of mounted police. For his anti-police tirade "Soldier Blue", Cope sampled Lenny Bruce's Berkeley Concert and mixed in samples of the Poll Tax riot itself . The song was later re-mixed by Disposable Heroes of Hiphopricy's Michael Franti, who also provided a rap for the new mix. However, when Island Records refused to release the record as being too overtly political, another argument ensued. Many of the songs on Peggy Suicide also reflected Cope's hatred of organized religion, and his increasing interest in the occult, animal rights, paganism, women's rights, the goddess and ecology. In 1992, Cope released another double album, the fiercely anti-Christian Jehovahkill. While the lyrics of such songs as "Poet is Priest", "Julian H. Cope", and the single "Fear Loves This Place" were again highly critical of the Church, much of the music on Jehovahkill reflected his teenage fascination for both Detroit hard rock and a more electro-acoustic based Krautrock. However, the contents of Jehovahkill were too much for Island Records, who dropped Cope the same week that his three shows sold out at London's 1800 capacity Town & Country Club. The press mounted an outcry at Island Records' decision, NME featuring him on their front cover under the headline 'Endangered Species' and Select magazine started a campaign to have Cope re-signed. Cope refused to comment because he was engaged in a tour of the Highlands and Islands of Scotland.
In the mid-1990s, Cope signed with Rick Rubin's Def American label, releasing Autogeddon (1994) and 20 Mothers (1995), spawning the single "Try, Try, Try", accompanied by two Top of the Pops performances. He was dropped by the label when he refused to visit the USA. In 1996, Cope released the album Interpreter (Echo Records). Cope's ongoing battle with those he referred to as "greedheads" eventually saw him turn his back on the music industry from this point onwards.