By 2000, the album had acquired a cult following; it was re-released and Bunyan recorded more songs, beginning the second phase of her musical career after a gap of thirty years.

[10] In London the following year, an actress friend of her mother's introduced her to The Rolling Stones' manager, Andrew Loog Oldham,[11] who signed her up to fill the gap left by Marianne Faithfull, who had recently left the label, and gave her a Mick Jagger/Keith Richards song to record, "Some Things Just Stick in Your Mind".

[6] Her distinctive vocal appeared on "The Coldest Night of the Year" by Twice as Much on their second and final LP, That's All, released by Oldham's Immediate Records in 1968.

In the spring of 1967, Bunyan left her job in a veterinary practice in London and set off with guitar and dog[11] to reconnect with a rebellious art student, Robert Lewis, she had met two years previously, with whom she was later to have three children.

"[6] In the harsh winter of 1968, Bunyan took a break from the journey in the Lake District and went to the Netherlands to try an unsuccessful tour performing in pubs and bars.

[14][11] Bunyan and Lewis resumed their pilgrimage northwards in March 1969, surviving on very little, and reached the Scottish highlands and finally the island of Skye, where they found that the "Renaissance community" had dissolved and there was nowhere for them to live.

They settled instead on the nearby island of Berneray, where Bunyan recalled being inspired by the spartan lives of the old women who befriended them, one of whom sang ancient songs to them in Gaelic and "made up stories to tell visiting Scottish folklore collectors.

"[11][6] In late 1969, Bunyan returned briefly to Boyd in London and recorded fourteen songs for her first LP over a six-week period in his Sound Techniques studio, with assistance from guitarist Simon Nicol and violinists Dave Swarbrick of Fairport Convention and Robin Williamson of The Incredible String Band, and string arranger Robert Kirby.

[11] She left Berneray with Lewis in April 1970 and returned briefly to London in an unsuccessful attempt to resume her musical career.

"[15] Disappointed, Bunyan left the music industry in 1971 and moved with Lewis for a few months to The Incredible String Band's Glen Row cottages in the Scottish Borders, then walked to the west coast of Ireland and returned to Scotland.

[16] In 2000, Just Another Diamond Day was re-released on CD with bonus tracks and introduced Bunyan's music to a new generation of folk artists such as Devendra Banhart and Joanna Newsom.

In 2002, she was invited by Piano Magic musician Glen Johnson to sing guest vocals on his song "Crown of the Lost", her first recording in over thirty years.

[20] The album, produced by composer Max Richter, featured many of her contemporary followers including Banhart, Joanna Newsom, Adem, Kevin Barker of Currituck Co, Otto Hauser of Espers and Adam Pierce of Mice Parade, and was well received.

[citation needed] In the autumn of 2006, Bunyan assembled an ad hoc band and embarked on a brief North American tour, with performances in Canada and the US.

She also provided vocals on three songs for the debut solo album of former Jack frontman Anthony Reynolds, British Ballads.

[24] In October 2008 a feature documentary about her, Vashti Bunyan: From Here To Before, directed by Kieran Evans, had its world premiere at the Times BFI London Film Festival.

I neither read nor write music, nor can I play piano with more than one hand at a time, but I have loved being able to work it all out for myself and make it sound the way I wanted.

[28] In 2023, she was invited by singer-songwriter Lail Arad to perform alongside Emeli Sande, Sam Amidon, Eska and This Is The Kit in a tribute concert at London's Roundhouse in April 2024 to celebrate Joni Mitchell's 80th year.

It included nine previously unheard home demos from the 2005 sessions with producer Max Richter and a live recording from a 2006 concert in Los Angeles.