Born into one of the most prestigious Austrian noble families, the House of Harrach, Aloys Thomas was the fourth son of Count Ferdinand Bonaventura I von Harrach and his wife, Countess Johanna Theresia von Lamberg, daughter of Count Johann Maximilian von Lamberg, Austrian diplomat and courtier.
From 1715 to 1742 he acted as 'Landmarschall' in Lower Austria, and from 1728 to 1733 as viceroy of Naples, from where he gathered numerous art pieces (Gallery in Rohrau).
From 1734 to his death Count Harrach was a member of the Secret State Conference (Geheime Staatskonferenz) in Vienna.
His oldest son, Count Friedrich August von Harrach-Rohrau, was interim governor of the Austrian Netherlands, and his youngest son, Ferdinand Bonaventura II von Harrach, governor of the Duchy of Milan.
Joseph Haydn's mother, Maria née Koler, once served as a cook in his palace.