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A brother of William Simson RSA, whose work he is often seen to emulate, George Simson came to Edinburgh in 1812 where he began his career as a printer with the 'Edinburgh Advertiser' newspaper before turning his attention to art.

In 1826 he and his brother David were appointed to the staff of the Edinburgh Drawing Institution which had opened the previous year in premises at 19 Hill Street, and continued there until early in 1831. George was appointed first Principal and David as second Assistant Master. In connection with the Drawing Institution George travelled to Paris to secure materials. William left for London prior to 1831 and on George's resignation he was succeeded as Master by Arthur Perigal snr, father of Arthur Perigal RSA.

George continued to teach, establishing the New Drawing Academy with his brother David round the corner from Hill Street and again on an upper floor, at 53 North Frederick Street. The New Drawing Academy operated an almost identical model as that of the Edinburgh Drawing Institution but introduced classes in modelling, led by David, and in life drawing, under the tutelage of George.

His Obituary in 'The Scotsman' newspaper of 1862-03-12 suggested that "As a teacher of drawing and painting, Mr Simson 's influence on our younger artists has been perhaps greater than that of many more illustrious professors of the art."

He also made at least one other overseas trip taking a summer sketching tour to Madeira which also saw him visit Portugal.

He produced figure paintings and landscapes in oil and chalk.

He was one of the original associates of the RSA in 1826 resigning soon after and rejoining the RSA as a member in 1929. He exhibited at the RSA Annual Exhibitions from 1830 until 1862.