Several medium and large pore molecular sieves were synthesized by hydrothermal synthesis method and examined for methylation of 2-methylnaphthalene. All the molecular sieves show good crystallinity with pure phase under the condition used. The physical properties of the materials were measured by the BET sorption method. The synthesized materials show microporous nature with typical type-I isotherm. However, BEA and MCM-22 shows slightly mesoporous characteristics with hysteresis loop. The activity of the molecular sieves catalysts for methylation of 2-methylnaphthalne decreases in the following order: Y=BEA>MCM-22>ZSM-5>SAPO-5. The rapid deactivation occurred in Y and BEA zeolite within 2 h time on stream (TOS). However, MCM-22 gave reasonable activity (50-40 % conv) with more stable performance. The SAPO-5 and ZSM-5 shows poor activity. The selectivity ratio of 2,6-DMN/2,7-DMN decreases in the order of SAPO-5>BEA=Y>MCM-22>ZSM-5.