A method for generating a bifunctional organolanthanide (III) initiator in situ from a (meth) acrylate monomer and a divalent samarium precursor,(C5Me5) 2Sm (1) or (C5Me5) 2Sm (THF) 2 (2), is described. This process involves one-electron transfer from the Sm (II) species to monomer, forming radical anions which couple to give a bimetallic samarium (III) enolate that acts as a bisinitiator for living polymerization. Well-defined, highly syndiotactic ABA ...