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Elizabeth Harris, nee Rees-Williams, died at the Chelsea and Westminster Hospital at 11.10pm on Good Friday after a long illness.
The daughter of the first Baron Ogmore, a Labour Cabinet minister in the 1945-51 Attlee Government, was married to former Tory minister Jonathan Aitken.
The one-time Rank starlet was previously married to actor Richard Harris, with whom she had three sons Damian, Jared and Jamie, who are all Hollywood-based actors or directors.
She was also formerly married to actor Sir Rex Harrison and Peter Aitken, the cousin of her widower.
She was the author of the memoir Love, Honour And Dismay published in 1976.
Mr Aitken, now a prison chaplain, will still lead the Easter Sunday service at HMP Pentonville in accordance with his late wife’s wishes.
Her funeral will be held on a date to be announced at St Matthew’s, Westminster.