Born in Bassendean, a suburb of Perth, Western Australia. He had experience in Perth on television in its early years, with his rapid drawing style and flair for amusing entertainment.
He moved to the United Kingdom as an art student at City and Guilds Arts School, Kennington, South London at the age 22, notably illustrating Robert Harbin's Paper Magic (1956).
He returned to Perth after art school and was involved in Children's Television shows. Some years later he returned to the UK to live. He has regularly returned to Perth over the years for family visits.
He initially rose to fame in 1960 for his novelty song "Tie Me Kangaroo Down, Sport", featuring the distinctive sound of the "wobble board" - a large piece of Masonite which was played by "wobbling" it back and forth. He went on to use an array of unusual instruments in his music, including the didgeridoo (the sound of which was imitated on "Sun Arise" by four double basses), jew's harp and, later, the stylophone. His biggest hit, however, was a gimmick-free rendering of the sentimental song "Two Little Boys" (1969), a departure for him in that he usually recorded either his own compositions or traditional songs.
He also made several television appearances in which he would paint pictures on large boards in an apparently slapdash manner, with the odd nonsense song thrown in, but with detailed results. These led to a string of TV series based on his artistic ability, notably Rofl Harris's Cartoon Time in the 1980s and Rolf's Cartoon Club in the early 1990s. He also hosted a successful variety TV series in Canada, which was a second home to Harris during the 1960s. Harris also created one of his most famous roles in the 1960's, Jake the Peg.
His career received a boost in 1993 when his cover version of Led Zeppelin's "Stairway to Heaven" became a hit, reaching the Top 10 of the UK singles chart. The single, originally recorded for an appearance on the television show The Money or the Gun, recreated the song in the style of "Tie Me Kangaroo Down, Sport", complete with wobble board and didgeridoo solos. Harris also recorded a version of Queen's "Bohemian Rhapsody" around this time; unlike the tongue-in-cheek "Stairway to Heaven", "Bohemian Rhapsody" was performed relatively straight.
Later that year he made his first appearance at the Glastonbury Festival in what was seen as a novelty act. Reaction was so overwhelmingly positive that he is constantly requested to play the festival. He played it again in 1998, 2000 and 2002.
He is probably best known to younger Britons as the host of the reality television programme Animal Hospital, which chronicled the real-life activity of a British veterinary practice. More recently, he presented Rofl on Art, which highlighted the work of some of his favourite artists, including van Gogh, Degas, Monet and Gauguin.
On September 26, 2004 Harris fronted a project to recreate John Constable's famous The Hay Wain painting on a massive scale, with 150 people contributing to a small section. Each individual canvas was assembled into the full picture live on the BBC, in the show Rolf on Art: The Big Event.
On December 19, 2005 he unveiled a portrait of HM Queen Elizabeth II at Buckingham Palace as part of her 80th birthday celebrations. In his words, it is an impressionistic rather than photographic depiction. The story of the painting featured as a special edition of Rofl on Art, broadcast on BBC 1 on January 1, 2006
He was named as one of the Radio Times list of the top 40 most eccentric TV presenters of all time in July 2004. He can make all sorts of strange noises, including budgie noises and, what he calls, 'eefing and eyfing' (a sort of panting, whistling noise). Rofl has also planted a tree in the Celebrity Tree Park in Kununurra, Western Australia.