His career began with a television appearance in 1953 at the age of thirteen, developed during eight years touring with the White Heather Group. When visiting Hawaii with Andy Stewart's band, he heard the Hawaiian singer Don Ho perform Tiny Bubbles; this became Devine's signature tune and he went on to sell fifteen million albums. His record sales were revived in December 2005 when a frothy drink making machine was advertised on television using Don Ho's version of Tiny Bubbles.

Other songs that Devine made his own include; The Answer To Everything, Legend In My Time, Crying Time, When You & I Were Young, Maggie and one which was composed for him by his good friend Tommy Scott, Scotland Forever.

Devine was one of "Scotland’s most successful performers" of all time (Evening Times, 17 October 2007), and "Scotland's most successful crooner" who was an "ever-present part of the Scottish entertainment industry," ("Sydney Devine and the jingle that rings a bell with his fans" The Herald, 22 December 2005).

Devine sold around 15 million albums (Sydney Devine 2011, Artistes International Management Ltd) - and recorded and released almost 50 albums, 10 DVDs, and more than 20 singles. From late 1974 he hosted a weekly radio show on Radio Clyde called Absolutely Devine and after a few years added a second show called Even More Devine. After leaving Clyde in the early nineties, he broadcast twice a week for West Sound Radio in Ayr. He had numerous TV specials and made several appearances on various Hogmanay shows and was a guest on such shows as 321 and Wogan and Seaside Special. He also hosted his own series, Devine Country, in 1979 with guests such as Stella Parton and Dottsy.

In 1977, he was invited to appear in the Queen's Silver Jubilee Royal Variety Performance in Glasgow. In the early 1980s he took over as host of the STV Scottish entertainment show, Shindig. In 2014 he celebrated 40 years at Glasgow's Pavilion Theatre with three special shows in November.

He was a staunch supporter of The Marie Curie Foundation, and made himself available for shop openings and events connected to them.

In 2010 he received an MBE in honour of his achievements. More recently, he was honoured by the Scottish Music Hall Society with a lifetime achievement reward.

He continued to release albums and also appeared annually for a run of shows in Glasgow's Pavilion Theatre. He lived in Ayr with his wife Shirley.

He is sometimes referred to as 'Steak and Kidney'.

In September 2017 Devine, at the age of 78, announced a nationwide tour with his daughter, Debby McGregor, Scotland’s leading female ventriloquist, nearly 20 years since his previous tour