We have shown that zeolite microcrystals can be readily organized in the form of uniformly oriented monoand multilayers on various substrates by well-defined chemical linkages based on covalent, ionic, and hydrogen bondings between the microcrystals and the substrates. This finding establishes the fact that micrometer-scale building blocks can be readily organized into organized entities through interconnection of the surface-tethered large number of functional groups. Since zeolite crystals have highly regular and uniform nanochannels and nanopores within them, the resulting mono and multilayers of zeolite microcrystals bear great potential to be utilized in various novel applications.