Bimetal cobalt nickel phosphate CoVSB-1 molecular sieves with the yield of about 88wt% have been synthesized rapidly in 4h at 443K under hydrothermal conditions. About 32.3 and 23.7wt% of ammonia gases can be adsorbed by VSB-1 and CoVSB-1, respectively, after being activated for 20min at 373K. Compared with the related adsorption amount of 17.5wt% for zeolite NaA, their adsorption amounts are very high, which may be due to the large pore diameters of 0.9nm, high surface areas (ca. 134 and 156m 2 /g for VSB-1 and CoVSB-1, respectively), suitable P–OH acidic activities, and a large amount of frameworks transition-metal nickels and/or cobalt coordination centers. The possible chemisorption mechanism could be deduced through the XRD patterns, FT-IR and UV–Vis spectra analytic results.