Zeolite materials with oriented macroporous and/or mesoporous structures hold promise not only for advanced catalysis and separation but also advanced applications such as medicines, photonics, photoelectronics, and other emerging nanotechnologies. Here we present a simple route for the generation of the oriented macropores in zeolite crystals through the direct disassembly of zeolitic building blocks formed during the crystal growth process by NaOH. The formation of the oriented macropores was predetermined by the generation of Na+ and OH− ions in zeolite crystals. NaOH amount in the initial gel was controlled at a high level to induce these ions into zeolite crystals by promoting the aggregate growth. The active Na+ and OH− ions released from the coalescence of the aggregates could dissolve the less stable crystalline domains or crack the T–O–T bonds along the crystal lattice planes resulting in the disassembly of the zeolitic building block and the formation of the oriented macropores. The zeolite product exhibits a monolithic morphology composed of mordenite (MOR) crystals with c-axis-aligned macrochannels. The monolith and oriented macroporous architecture with its good hydrothermal stability could make it as an interesting material platform for fundamental studies of the structure–properties correlation and the special applications.