The news of his death was reported on 'Captain Scarlet' creator Gerry Anderson's website, reported Contactmusic.
"We are very sorry to report that Francis Matthews, best known to Gerry Anderson fans as the voice of the indestructible puppet hero Captain Scarlet, has died aged 86," he wrote.
Matthews is survived by three sons from late wife Angela Browne.
He voiced the puppet in the science-fiction television series which ran between 1967 and 1968.
From 1969 Matthews also played Paul Temple in the BBC detective series of the same name.
Born and raised in York, Matthews began his acting career at the Leeds repertory theatre before serving in the Royal Navy.