Bain was born in Lerwick, Shetland. In the early years of his career, he was—briefly and unofficially—part of the band The Humblebums with Gerry Rafferty, Billy Connolly and Tam Harvey. He was one of the members of the band "Gordon Hank and the Country Ramblers", which also included Gordon Smith, Ian Stewart and Jack Robertson in 1967 and was based in Shetland.
He became nationally prominent as a founding member of The Boys of the Lough, a Scots-Irish folk group, with whom he played for over 30 years.
Simultaneously, Bain pursued a solo career in collaborative and television projects with Pelicula Films director Mike Alexander and producer Douglas Eadie, working on several international television series: The Down home Recordings (which described how fiddling music spread from Scotland and Ireland to America), The Shetland Sessions (recorded at the Shetland folk festival in 1991), Aly Meets The Cajuns, and six series of the Transatlantic Sessions.
In 2000, Bain played at the funeral of the Scottish first minister Donald Dewar.
In 2006, a television programme celebrating Bain's 60th birthday was broadcast by the BBC, documenting his life and works. The same year, Bain was inducted into the Scots Traditional Music Hall of Fame.
In 2009, Bain collaborated with Nicola Benedetti to create a television programme for BBC Scotland: When Nicola Benedetti Met Aly Bain, broadcast the same year.
In 2012, Bain and Cunningham celebrated their 25th anniversary of touring as a fiddle and accordion duo. Bain also tours with Swedish multi-instrumentalist Ale Möller (with whom he has recorded two albums) and with American old-time fiddler, singer, guitarist and banjo player Bruce Molsky; as a trio, they released their first album in 2013.
Honours and awards
Bain has received many honours for his services to music.
In 1989, he received a Silver Disc from the Record Industry Association for his Aly Meets the Cajuns recording. A further Silver Disc followed in 1991 for The Pearl, recorded on his own Edinburgh Record Label, Whirlie Records.
In 1994, he was awarded the MBE for his musical accomplishments.