He also sat as Liberal Member of Parliament (MP) for two separate five-year periods: for Coventry from 1880 to 1885, and for Bristol East from 1895 to 1900.

Lord Winterstoke was a keen supporter of the arts, serving as President of what is now the Royal West of England Academy (RWA) from 1898 until his death in 1911 and donating the money to create Bristol City Art Gallery, whose facade bears the inscription "The Gift of Sir William Henry Wills to his Fellow Citizens 1904".

[5] A zealous nonconformist by personal conviction as well as by family tradition, he actively engaged in the affairs of the free churches.

He joined the board of the Dissenting Deputies, was a trustee of the Memorial Hall in London, and took a practical interest in the refoundation of Mansfield College, Oxford in 1886.

A portrait of Lord Winterstoke hangs in the Middle Common Room of Mansfield College, Oxford.