Harlay is a French surname. Notable people with the surname include:
- Nicolas de Harlay, seigneur de Sancy (1546-1629)
- Christophe de Harlay, Count of Beaumont (1570-1615) French ambassador to England
- Achille Harlay de Sancy (1581-1646)
- François II de Harlay Archbishop of Rouen (1614-1651)
- François de Harlay de Champvallon (1651-1695)
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