The company had been planning to move beyond Brighton for some time and the new store, due to open after Easter, would mark the end of a turbulent year for the business, said Taj director Amir Khan.
"We are on the up and have been looking to expand in the Crawley area for a while," he said.
Taj chose the centre of Crawley because there was a good demographic fit, he said. "A lot of customers come down from Crawley to our Brighton store already. We are just meeting local demand," he said.
The new outlet will provide the same specialist and organic produce as its Brighton store and is due to open next month after planning permission is secured for modifications to the former charity shop.
Last March, the grocer's parent company, Taj Mahal Natural Food Ltd, went into administration. At the time it owned two stores in Brighton and these were bought by Taj Mahal International Foods, which has the same owners, a few days later. However the new company closed the store in the Kemp Town area in November.
Last month, squatters moved into the vacant Taj property in protest against a Sainsbury's Local opening there as part of a "Sabotaj" campaign. Taj dismissed rumours last week it would reopen the store if Sainsbury's failed to secure an alcohol licence for the premises.