A series of SAPO-11 zeolites with different Si contents were prepared by hydrothermally synthesized method. They were characterized by ICP, XRD, SEM, FT-IR, N2 adsorption-desorption, NH3-TPD and 29Si MAS NMR, and evaluated by the methylation of naphthalene with methanol to 2,6-dimethylnaphthalene (2,6-DMN). According to XRD and SEM results, the crystallinity of SAPO-11 sample increased with increase of the Si content until the SiO2/Al2O3 ratio was up to 0.2. However, a reduction in the crystallinity was observed with further increase of the Si content of the synthesis. N2 adsorption-desorption results showed that all the samples possessed micropores and secondary mesopores. SAPO-11 sample with SiO2/Al2O3 ratio of 0.2 exhibited the largest secondary mesopores size distributions. NH3-TPD and 29Si MAS NMR showed that the Si content was incorporated into the framework affecting not only the acid sites but also the acid strength of SAPO-11. SAPO-11 with SiO2/Al2O3 ratio of 0.2 presented the high catalytic performances for the methylation of naphthalene, which was mainly attributed to the amount of secondary mesopores in the SAPO-11 zeolite.