Polymeric analogs of tetramethylurea were prepared by free-radical polymerization ofN,N,N'-trimethyl-N'-p-vinylbenzylurea and copolym-erization of this monomer with styrene. These polymers are soluble in toluene and have the ability to extract alkali metal ions such as lithium, sodium, and potassium. Moreover, these polymers act as phase-transfer catalysts for typicalSN2 reactions, although the monomeric analogs tetramethylurea andN,N,N'-trimethyl-N'-benzylurea do not. A plausible mechanism for these catalytic reactions is proposed.