The first recorded reference to the name of Airthrey is in a Charter of King David of Scotland, which must have been granted prior to 1146. The Airthrey Estate appears to have been held by the Crown until 1370, when it was granted to Sir John Herice, Knight Keeper of the Castle of Stirling.
The land then passed into the hands of William, Lord Graham of Kincardine, to recognise the gallantry he showed at the Battle of Sauchieburn. After being made Earl of Montrose, he was killed at the Battle of Flodden Field in 1513.
Airthrey remained in the Montrose family until the fifth Earl was executed at Edinburgh in 1650 for his support of the royalist cause. By then, the manor house of Airthrey had been burned to the ground by Covenanters under the Marquess of Argyll.
The estate was purchased by John Hope of Hopetoun in 1678, then passed in 1706 to Ralph Dundas, whose son John Dundas built the house at Airthrey in 1748. Next, the estate was bought by Captain Robert Haldane of Plean in 1759, and his great-nephew Robert commissioned the extravagant design by Robert Adam that forms the southern half of the current building.
Robert Haldane also built the stone wall that extends nearly four miles round the edge of the estate, and was responsible for the early development of the landscape, including the creation of the loch. However, once the house was built he sold it, with the estate, in 1798 to Sir Robert Abercrombie for £46,000. Sir Robert immediately set about improving the estate, and was responsible for moving the village of Logie to a new site in Causewayhead, and also "discontinued the village of Pathfoot".
The estate continued to be held by members of the Abercrombie family until 1889 when it was bought by Donald Graham for £75,000. He built a large addition on the north side of the castle in 1891, at a cost of £15,700 with impressive interior features such as a carved oak panelled hall, alabaster plaques, white marble fireplaces and intricately carved Eastern doors.
It remained with the Graham family until it was handed over to the Secretary of State for use as a maternity hospital, and many hundreds of children were born here between 1939 and 1968.
By that time, the University of Stirling had come into being, and the Castle was taken over in 1969 to become an integral part of University life. Initially it housed administrative and social functions, but is now primarily used for teaching by the School of Law.