A method of increasing the amount of acid sites, especially Bronsted acid sites, on the surface of Hβ zeolite is reported. The Hβ samples were prepared through NH4NO3 solution ion exchange, citric acid treatment, and 823 K calcination from as-synthesized zeolite beta using sodium aliminate or pseudoboehmite as the aluminum source, and were characterized by NH3-TPD, pyridine-IR, 29Si MAS NMR, and 27Al MAS NMR. The surface properties of Hβ zeolite changed after the citric acid treatment as follows: acid strength decreased, total acid amount increased, Bronsted acid sites increased and Lewis acid sites remained unvaried. The citric acid treatment of zeolite beta may have functions of dealumination at a Si(2Al) site and realumination at a Si(0Al) site.