Though she was appointed a member of the board of the Astor Foundation soon after her marriage, upon Vincent Astor's death in 1959, she took charge of all the philanthropies to which he left his fortune. She served as a Trustee of the Metropolitan Museum of Art and chaired the Visiting Committee of the Metropolitan's Department of Far Eastern Art; she is credited with the idea for a Chinese garden courtyard, the Astor Court, in the Metropolitan. In addition, Astor served as a member of the Metropolitan Museum of Art's 100th Anniversary Committee and hosted the Metropolitan's Centennial Ball.