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After splitting from Williams, Samson met Pink Floyd singer and guitarist David Gilmour, whom she married in 1994 during Pink Floyd's Division Bell tour. Her son Charlie was adopted by Gilmour and they have three other children: Joe, Gabriel, and Romany.
She has also written short stories for BBC Radio 4 and has had a collection published Lying in Bed (Virago 1999) and a novel, Out of the Picture (Virago 2000), as well as contributing pieces and stories to many other books and publications including Gas and Air (Bloomsbury 2003), Girls Night In (Harper Collins 2000), A Day in the Life (Black Swan 2003), and The Just When Stories (Beautiful Books 2010). Samson's collection of stories, Perfect Lives, was published in November 2010 by Virago Press. Her novel, The Kindness, was published in 2015.
Samson is credited as a co-writer on seven of The Division Bell's 11 tracks, and, with the retrospective credit given to Clare Torry for her vocals on "The Great Gig in the Sky", she is one of only two female co-writers of any Pink Floyd songs. She also wrote lyrics for Gilmour's 2006 album, On an Island, and made a guest appearance on piano and vocals. She contributed lyrics to "Louder than Words", the only track on Pink Floyd's 2014 release, The Endless River, to contain any sung lyrics. Samson has also contributed lyrics to half of the tracks on Gilmour's latest album, Rattle That Lock (2015), some of which were inspired by Paradise Lost, an epic poem by John Milton.
In 2018, Samson was made a Fellow of the Royal Society of Literature.
Samson's novel, A Theatre For Dreamers, was published on 2 April 2020 by Bloomsbury Circus. The novel entered the Sunday Times Bestsellers Chart at number two.