Nanocrystalline zeolites are porous nanomaterials with crystal sizes of less than 100 nm that possess unique external and internal surface reactivity. Nanocrystalline zeolites, such as silicalite, ZSM-5 and Y, were synthesized and extensively characterized by powder X-ray diffraction, nitrogen adsorption isotherms, dynamic light scattering, and electron microscopy. Spectroscopic characterization of the nanocrystalline zeolites by FTIR and solid-state NMR provided detailed structural information about internal and external surface sites. The nanocrystalline zeolites were also used as building blocks to form larger, hollow zeolite structures with encapsulated metal or organic species. The surface properties of nanocrystalline zeolites and hollow zeolite structures were tailored through functionalization of surface silanol groups. Applications of nanocrystalline zeolites and zeolite structures in the selective catalytic reduction of NO_x and the photoreduction of Cr(VI) to Cr(III) in aqueous solution were investigated. The unique properties and reactivity of nanocrystalline zeolites and the potential for future applications of these materials will also be discussed.