The paper reports the preparation of two series of nanosized (150-350 nm) ZSM-5 zeolite crystals with a Si/Al molar ratio of 70 to 144 by a template method. The prepared catalysts are distinctive in their mostly intercrystalline macroporosity and random architecture of transport channels formed as a result of the utilization of a high-molecular-weight template represented by suspended or powdered polystyrene particles about 250 nm in size. The crystallinity and the size and packing of the particles depend on the method of template introduction into a precursor mixture. The samples of both series were tested in an n-hexane cracking reaction, and the comparative assessment of their catalytic properties in terms of n-hexane conversion degree and selectivity for alkane, olefin, and isoalkane products is also summarized in the paper.