His other work includes graphics for rock group Pink Floyd, particularly on their 1979 album The Wall, its 1982 film adaptation, and tour (1980–81), as well as the music video for "Welcome to the Machine".

[8] After briefly working in advertising, a profession he grew to dislike intensely, Scarfe's early caricatures of public figures were published in satirical magazine Private Eye throughout the 1960s and 1970s.

His decision to work for the Daily Mail led to his estrangement from fellow cartoonist Ralph Steadman, alongside whom he had studied art at East Ham Technical College.

Scarfe was approached to work with Pink Floyd after Roger Waters and Nick Mason both saw his animated BBC film A Long Drawn Out Trip.

[13] As well as the artwork, Scarfe contributed 15 minutes' worth of elaborate animation to the film, including a sequence depicting the German bombing campaign over England during World War II, set to the song "Goodbye Blue Sky".

The book contains contributions from Floyd members Roger Waters, Nick Mason, and David Gilmour, as well as director of the film, Alan Parker.

Honoring English comedians, the stamps feature Scarfe caricatures of Tommy Cooper, Eric Morecambe, Joyce Grenfell, Les Dawson and Peter Cook.

[20] [citation needed] In 2003 Scarfe collaborated with the National Portrait Gallery and BBC Four to make caricatures of a number of famous Britons, to depict (along with guest commentary) their heroic and villainous attributes.

Amongst the over 30 portraits he depicted included caricatures of Henry VIII, Winston Churchill, Queen Elizabeth I, Pete Best, Richard Branson, Adam Smith, William Blake, The Beatles, Agatha Christie and Diana, Princess of Wales.

[citation needed] In its edition of 27 January 2013 (Britain's Holocaust Memorial Day), London's Sunday Times published a cartoon by Scarfe depicting Israel's Prime Minister Benjamin Netanyahu paving a wall with the blood and bodies of Palestinians, captioned "Israeli elections—will cementing peace continue?

"[21] The cartoon's timing and content was criticised by groups including the European Jewish Congress and the Board of Deputies of British Jews, with accusations of antisemitism leveled against Scarfe.

[25][26] The newspaper's proprietor, Rupert Murdoch, apologised for the cartoon on Twitter, and acting editor Martin Ivens promised to be more vigilant in future.

[32] In October 2013 Scarfe donated his time to decorate one of the large Wallace & Gromit statues to be auctioned for the Bristol hospital charity that was featured live on the BBC.