A generalized synthesis of high-quality, mesoporous zeolite (e.g., MFI-type) nanocrystals is presented, based on a biomass-derived, monolithic N-doped carbonaceous template. As an example, ZSM-5 single crystals with desirable large-diameter (12-16 nm) intracrystalline mesopores are synthesized. The platform provides scope to optimize template dimensions and chemistry for the synthesis of a range of micro-/mesoporous crystalline zeolites in a cost-effective and highly flexible manner.