A route to synthesize ZSM-5 crystals with a bimodal micro/mesoscopic pore system has been developed in this study; the successful incorporation of the mesopores within the ZSM-5 structure was performed using tetrapropylammonium hydroxide (TPAOH)-impregnated mesoporous materials containing carbon nanotubes in the pores, which were encapsulated in the ZSM-5 crystals during a solid rearrangement process within the framework. Such mesoporous ZSM-5 zeolites can be readily obtained as powders, thin films, or monoliths.