The results of synthesis and packing of crystallized iron-containing nanosized zeolites of MFI structure in dense and loose structures having different textural properties are reported. Data on the formation of additional meso- and macropores immediately during zeolite crystallization using polystyrene microspheres in the form of an aqueous suspension (latex) and as a dry template of closely packed particles are also presented. Advantages and disadvantages of these procedures for preparing hierarchical iron-containing MFI structure zeolites have been compared. Values of the external surface area and the total pore volume of hierarchical Fe-silicalites are significantly higher than those for a reference sample. Using the polymer template to synthesize the hierarchical material consisting of zeolite nanocrystals makes it possible can significantly reduce the synthesis time and simplify the preparation procedure.