This Account summarizes various methods of organizing zeolite microcrystals into two-dimensional functional entities such as monolayers, multilayers, and patterned monolayers on various substrates and three-dimensional functional entities such as microballs and protein-zeolite composite fibrils. In the case of monolayer assembly, various types of linkages and substrates, factors that govern the rate, degree of coverage, degree of close packing, degree of uniform orientation, and average binding strength between each crystal and the substrate are described. The current and future applications of the organized products are also discussed.