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A new type of NZP family compound CaZr4(PO4)6 was synthesized by sol-gel method and coprecipitation method respectively, and the acidity of CaZr4(PO4)6 was modulated by doping aluminum. The phase and pore structure of the samples were characterized by X-ray diffraction (XRD) and N2 adsorption-desorption, the acid catalytic activity of CaZr4(PO4)6 doped by Al were investigated by using alpha-pinene isomerization as probe reaction. The results show that CaZr4(PO4)6 doped with Al element synthesized by sol-gel method have regular mesoporous structure and weak strength acid site, therefore the catalytic activity on these samples for alpha-pinene isomerization is higher than that on the Al doping samples prepared by coprecipitation method.