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Abstract: We applied molecular crowding, which is known as a characteristic feature of molecular environments in cell, to synthesis of polymeric functional materials capable of molecular recognition. The synthesis was conducted by a crowding-assisted molecular imprinting technique, in which association of a template molecule and functional monomers is stabilized with the addition of crowding agents. Obtained polymers exhibited enhanced affinity and selectivity compared with polymers prepared in the absence of the crowding agents. The results suggest that molecular crowding would be useful for organic synthesis based upon molecular self-assembly and self-organization. (author abst.)