He was educated at Trinity College, Cambridge, and admitted to Gray's Inn on 12 November 1634. He lived at Newlands, Coventry, Warwickshire.
During the English Civil War he captained a Royalist troop of horse. The Yorkshire Royalist Composition Papers show him a "delinquent": in his petition he said that his estates had been sequestered and all his personal property plundered to the extent of £1500, and he could not pay his sister's portion as provided in his father's will, which was charged upon the rectory of Snainton, Yorkshire worth £55 a year. On 6 July 1649 his fine was remitted in return for his undertaking to pay £20 a year out of the revenue from the rectory to the Minister of Snainton and his successors.
He was knighted on 13 June 1660 for services to the Royalist cause. He was appointed a Page of the Privy Chamber to King Charles II and a Gentleman of the Privy Chamber in Extraordinary. Calendars of State Papers show him as one of the leading Warwickshire gentry responsible for ensuring payment of various taxes in the county and record deductions from the sums due in years of plague or when there were other special factors. He seems to have given up some or all of this responsibility in 1671: on 11 May 1671 Sir George Downing told the Commissioners of Excise that, on application from "Arthur Cailey", "the lease of the Excise of Warwickshire is to be in Mr. Purefoy's name only". This suggests Arthur Cayley was a joint lessee with Mr Purefoy.
In 1683 he was appointed a Deputy Lieutenant of Warwickshire.
He may be the 'Arthur Cale' whose burial is recorded at Exhall on 18 June 1698. In other sources his surname is sometimes spelt Caley, Cailey or Caly.
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