He contributed verses to the local newspapers and published some pamphlets, before leaving his native city in early life.

After a period of military service, he lived at first in Edinburgh but finally settled in London, where he gained a reputation as a writer and composer of songs and ballads.

Among his most fashionable and popular ballads, composed between 1830 and 1847, were Thou art gone from my gaze, Song of the roving gipsey, Constance; and later, between 1852 and 1862, with a stronger vein of melody, Minnie, Old friends at home, and the Robert Burns poem, The Jolly Beggars.

Linley's flowing style of composition was little suited to the stage, and his musical pieces produced at London theaters had small measure of success.

Linley died, after a lingering illness, at Kensington, London, on 10 September 1865, and was buried at Kensal Green Cemetery 5 days later.

One obituary stated, "The absence of the happy face and wit of George Linley from many a gathering of musical and literary men in London will be long felt as a loss not easily supplied.