He was the eldest of the 18 children[1] of Henry Overton Wills II (1800–1871) by his first wife Isabella Board.

His younger half-brother was Sir Frank William Wills, Knight, Lord Mayor of Bristol.

When the formation of Imperial Tobacco greatly increased the family’s wealth, various members began to contribute significant amounts of money to local causes.

[2] The most significant of these was announced in 1908 by his eldest son Sir George Alfred Wills, 1st Baronet (1854–1928), when he read a letter from his father promising £100,000 (about £10 million in today's money) to fund a university at Bristol if a royal charter for the purpose could be obtained within two years.

[3] In 1853 at Plymouth in Devon he married Alice Hopkinson (1827–1881), by whom he had issue including: He died on 4 September 1911 at Kelston Knoll and was buried in Arnos Vale Cemetery in Bristol, where survives his monument, together with many others of the Wills family.