It happened on Oct. 20 just before noon at CardVault by Tom Brady.
Authorities say after the man's credit card was declined, he manually bypassed the denial in the store's credit card machine without the employee's knowledge.
Police say he then left with approximately $9,710 worth of baseball and Pokémon cards.
No injuries were reported.
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The suspect was last seen headed south on Lafayette Street wearing all black and white sneakers and carrying a multi-colored bag.
The store is part of a chain backed by Tom Brady. There are locations in Dallas, Chicago, East Hampton, East Rutherford, Boston, Foxborough, Mashantucket, and a location in the Mall of America in Minnesota opens this weekend.
Anyone with information is asked to call the NYPD's Crime Stoppers Hotline at 1-800-577-TIPS (8477) or for Spanish, 1-888-57-PISTA (74782).