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He was the son of William Villiers, 2nd Earl of Jersey. Among other achievements, Villiers was a founding Governor of the Foundling Hospital, a charity which received its royal charter on 17 October 1739 to operate an orphanage for abandoned children in London.
On 23 June 1733, he married Anne Russell, Dowager Duchess of Bedford (c. 1704/1709 – 1762). She was the daughter of Scroop Egerton, 1st Duke of Bridgwater, and widow of Wriothesley Russell, 3rd Duke of Bedford. They had two sons, but only one survived them:
- Frederick William Villiers, Viscount Villiers (25 March 1734 – before 11 October 1742)
- George Bussy Villiers, 4th Earl of Jersey (1735–1805)
He commissioned the building of the previous Middleton Park, in Middleton Stoney, Oxfordshire.
- Mosley, Charles, editor. Burke's Peerage, Baronetage & Knightage, 107th edition, 3 volumes. Wilmington, Delaware, U.S.A.: Burke's Peerage (Genealogical Books) Ltd, 2003. Page 2096.
- thepeerage.com Retrieved 5 September 2009: William Villiers, 3rd Earl of the Island of Jersey
The Lord Cornwallis
| Justice in Eyre
south of the Trent
1740 – 1746
The Earl of Halifax
|Peerage of England|
| Earl of Jersey
1721 – 1769
|Peerage of Ireland|
| Viscount Grandison
1766 – 1769
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