From 1961 to 1966, he starred in the sitcom Marriage Lines with Richard Briers and Prunella Scales. De Souza had roles in the Hammer films The Phantom of the Opera (1962) and The Kiss of the Vampire (also 1962).
In 1965, he appeared as the lead in the Doctor Who story Mission to the Unknown – the only story ever broadcast in the series not to feature the Doctor in any capacity. In 1977 he played Sheik Hosein in the James Bond film The Spy Who Loved Me. He was solicitor "Bonny Bernard" in the first series of Rumpole of the Bailey (1978). In 1982 he appeared in the final Sapphire & Steel adventure as "The Man". He also appeared in the television version of After Henry (1989–90), Farrington and, earlier, took the part of Soveral (the Portuguese Ambassador to Britain) in Edward the Seventh (1975). One of his less-known works, was his role in The Golden Compass, in 2007, playing the Second High Councillor. In succession to the originator of the role, Valentine Dyall, he was The Man in Black on BBC Radio 4 between 1988 and 1992. de Souza played the role of Afonso in One Foot in the Grave One Foot in the Algarve (1993).
He joined the British soap opera Coronation Street as Colin Grimshaw, where he made his first appearance on 12 December 2008. His character died in May 2009.
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Edward de Souza Autograph - Doctor Who - Signed 10x8 Photo - Handsigned - AFTAL