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It joins stationery retailer Staples and outdoor pursuits store Cotswold, which have taken units of 3,500 sq ft and 8,000 sq ft respectively.
The listed building already has permission for 14 flats on its upper floors.
Richard Lewis, property director at TCS, said: “The building is well recognised throughout the city and due to its strategic location we didn’t want to limit the uses. We are confident that Pau Brasil can make good use of the building’s location and footfall.”
TCS acquired the building in 1997 and is also developing the ÂŁ250m