The company has taken the ground and basement which totals 1,003 sq ft on a 10-year full repairing and insuring lease.
This is the first site in the UK for the French chain, which will operate as a high end rustic bakery, with an ancillary retail element.
Aux Pains de Papy previously operated six branches across the South of France, which have now been sold.
Joshua Rose, Central London leisure agent, Shelley Sandzer said: “This is the first site for Aux Pains de Papy in London and will prove popular with the Midtown office crowd looking for well made, well presented delicacies.
"As consumers are becoming more discerning, there has been a demand for high end, quality bakeries, which Aux Pains de Papys certainly fills.”
The Esposito-family has over 70 years of experience and tradition in bakery with the tradition being started by Mathieu’s grandfather, Honoré Eposito in the South of France in 1948.
The company plans to open a further four sites in London by 2018.