After graduating from Oxford, Cayley took up residence in North Yorkshire where he engaged in farming. He also undertook studies in history, economics, and philosophy to supplement his "dead language" formal education. Caley became a "barrister-at-law" with membership in the Inner Temple. As a magistrate and barrister, his doors were always open for counsel. He promoted the Yorkshire and other agricultural societies as a speaker and writer. Thus, Cayley became well-known and highly respected by the farmers of his district, so much so that they called on him to represent them in Parliament. At the 1832 general election he stood for election in the two-member county constituency of North Riding of Yorkshire as an independent of Liberal sympathies and a friend of the interests of small agriculturalists, 'unassisted by the aristocracy on either side' and was elected a member of parliament, behind William Duncombe a Tory with major landholdings in the Riding, but ahead of John Charles Ramsden a former Whig MP for Yorkshire who had the support of the Whigs but was a West Riding industrialist. Cayley held the seat until his death in 1862, at the age of 59. As an independent member of Parliament, Cayley fought against "inequalities of taxation". He served on the Agricultural distress and Hand-loom weavers committees Cayley died of heart disease while making the arduous trip to London. The Farmer’s Magazine gave Caley a glowing obituary as a "farmers' friend", who "stood with the farmers, by the farmers, and for the farmers."
George John Cayley, a barrister educated at Eton and Trinity College, Cambridge. He had left-wing tendencies and in 1868 stood as the Working Man's candidate for Scarborough in the general election. He published several pieces of light verse, a book on electoral reform and the working classes, and a popular book about travels in Spain. The frontispiece of this book shows him with a magnificent mid-Victorian beard. He had a reputation as an accomplished metal-worker; in 1862 he and the painter George Frederick Watts designed the challenge shield for a national shooting championship at Wimbledon. He also was an accomplished tennis-player; he helped to develop several types of tennis racket, and wrote an article on the game for the Edinburgh Review in 1875. He had homes at Wydale Hall, Snainton, North Yorkshire and in Westminster. In 1860 he married Mary Anne Frances Wilmot ; they had three children:
* Hugh Cayley, educated at Trinity College, Cambridge, who lived at Wydale and married Rosa Louisa Violet, daughter of Johann Seelig of Hanover
*Arthur Cayley
*Violet Cayley, who took part in amateur theatricals at public theatres in Norfolk
Charles Digby Cayley, educated at Eton, who became a midshipman in the Royal Navy, was awarded a medal for his part in activities in the Levant, and drowned with a companion when a squall hit the sailing-boat they were in off Largs, Scotland.
