Robert Home was soon on the move again, travelling to London to enlist on 21 July 1760 as Surgeon to General Burgoyne's regiment the 16th (Light) Dragoons, who were preparing for action in Portugal during the Seven Years’ War. Leaving the rest of the family in Scotland, it is likely that Anne came south with her father, for at some point between then and April 1762, she became an intimate friend of an American, Alice Lee. The orphan daughter of Thomas Lee of Virginia, Alice had come to London in the early summer of 1760 to stay with her uncle, Philip Ludwell III. It is often said that the two girls were school friends, but as Alice was 24 at this time and Anne 19 or 20 this seems unlikely, although perhaps they attended music classes together. In London as in Edinburgh the musical activity of women was largely confined to private houses and although there were some concerts in the late 1750s and early 1760s, the great florescence of concert life would come later in the century. At this time however women could attend subscription concerts at Hickford's Rooms in Brewer Street for example, and at Mrs Cornelys’ Carlisle House in Soho Square, made deliberately exclusive by high charges. Anne could not have afforded the cost, though it is of course possible that she was invited by wealthier friends. There were also rather more light-hearted concerts in the summer at the Ranelagh, Vauxhall and Marylebone Gardens that young women like Anne and Alice might have been able to visit.

Anne may have lodged with one of her numerous relatives, or possibly at the boarding-house run by Anne and Peggy Elliot in Lisle Street, frequented by David Hume on his visits to London. This is not as fanciful as it appears as it is clear from a letter she wrote much later to Alice that both of them had been acquainted with him in the years before his visit to France in 1763. However, it is possible that Alice accompanied one of her brothers, Arthur Lee, to Edinburgh where he was studying medicine from 1761 to 1764 and encountered both Anne and David Hume there.