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Abstract: The synthesis of transition metal active sites by the molecular imprinting of polymerizable metal complexes into highly crosslinked organic polymers is described. The emphasis of this Account is on the synergy between the long-term goals associated with new catalyst development and the more short- term goal of addressing fundamental questions in coordination chemistry, particularly emphasizing stereochemistry and structure. An argument is presented that the latter is necessary for ultimately achieving the more difficult but more important goal of designer catalysts that achieve reaction selectivities and reactivities not obtainable with traditional homo- or heterogeneous catalysts