In 1839, he became first secretary of a committee formed by the Privy Council to administer the Government grant for public education in Britain.

He was a key figure in the foundation of the Girls' Public Day School Company and a member of its council until shortly before his death.

In 1842, he married Janet Shuttleworth (born 9 November 1817, half-sister of Marianne North), assuming by royal licence his bride's name and arms.

[10] His eldest son, Sir Ughtred James Kay-Shuttleworth (1844–1939), became a well-known Liberal politician, as MP for Hastings from 1869 to 1880 and for the Clitheroe division of Lancashire from 1885 to 1902, when he was created Baron Shuttleworth.

She was also introduced to Elizabeth Gaskell by the Kay-Shuttleworth's, when both women were invited to stay at their rented home in the Lake District in 1850.