We reported a perfect strategy for the fabrication of Cu-encapsulated hierarchical MEL zeolites by a simple post-desilication-recrystallization strategy. The Cu-encapsulated hierarchical MEL zeolites exhibited extraordinary selectivity in the liquid alkylation reaction of mesitylene and benzyl alcohol compared with hierarchical MEL zeolites, indicating that the additional Cu species located in the matrix of MEL zeolites can effectively inhibit self-etherification of benzyl alcohol. In addition, the selectivity of 2-benzyl-1,3,5-trimethylbenzene for the Cu-containing hierarchical MEL zeolites was in the order of H-MEL@Cu-26 < H-MEL@Cu-30 < H-MEL@Cu-47, which meant that the catalytic performance of zeolite catalysts can be modulated by tuning the acidity of zeolites, and a balance between the redox properties of Cu species and acidity of zeolites can be realized for the design of the ideal solid acid catalysts with desired catalytic performance.