An effective and rapid procedure to synthesize hierarchical MOR (Hi-MOR) nanosheets by self-assembly between subnanocrystals and organic templates was reported. The hierarchical pore systems provided a large quantity of Brønsted acid sites. Compared with conventional mordenite, Hi-MOR showed higher activity, xylene selectivity and longer catalytic life in the reaction of toluene disproportionation, thanks to its excellent diffusion from hierarchical structure. Graphical Abstract Hierarchical morednite (Hi-MOR) nanosheets were synthesized by self-assembly between subnanocrystals and organic templates.