Rayne and his wife divorced in 1960 and on 2 June 1965, he married Lady Jane Vane-Tempest-Stewart (a daughter of the 8th Marquess of Londonderry and sister of Lady Annabel Goldsmith) and they had four children: Natasha Deborah (b. 1966), Nicholas Alexander (b. 1969), Tamara Annabel (b. 1970) and Alexander Philip (b. 1973).
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In 1964 Darwin College, Cambridge was founded with support from the Rayne Foundation and a personal donation from Rayne himself, and this is acknowledged by the college in two notable ways: Firstly, on the college's coat of arms, which superimposes Rayne's coat of arms alongside that of the Darwin family's where the college gains its namesake.
In 2007, the Max Rayne School, a bilingual Hebrew-Arabic school was founded in Pat, open to all Jewish and Arab children in Jerusalem.
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