Wilmer died in hospital in Ipswich on Thursday after suffering from pneumonia, Roger Johnson, spokesman for the Sherlock Holmes Society Of London, confirmed, reported BBC.
"He was a great actor, he was a gentleman, he had a long and distinguished career," Johnson said.
Wilmer first appeared as Sherlock Holmes in 1964, with Nigel Stock as his Watson.
After he left the show he was replaced by Peter Cushing - but he retained his affection for the character throughout his career.
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And in 2012, at the very end of his acting career, he made a special cameo appearance in an episode of "Sherlock" as an irate old man at The Diogenes Club alongside current Sherlock, Benedict Cumberbatch.
The writer, producer and actor Mark Gatiss, who plays Sherlock's older brother Mycroft, shared a photograph of himself with Wilmer.
He tweeted: "An honour to have known dear Douglas Wilmer. A Sherlock for all seasons. The work was something, the man was all. RIP."