The reaction between [CdBr 2 ·4H 2 O] and anhydrous [ZnCl 2 ] with N,N'-bidentate N-(pyridin-2-ylmethylene)-cyclopentanamine (impy) in ethanol yields dimeric [(impy)Cd(µ-Br)Br] 2 and monomeric [(impy)ZnCl 2 ] complexes, respectively. The X-ray crystal structure of Cd(II) and Zn(II) complexes revealed that the cadmium atom in [(impy)Cd(µ-Br)Br] 2 and zinc in [(impy)ZnCl 2 ] formed a distorted trigonal-bipyramidal and tetrahedral geometry, respectively. Both complexes showed moderate catalytic activity for the polymerisation of methyl methacrylate (MMA) in the presence of modified methylaluminoxane (MMAO), with polymethylmethacrylate (PMMA) syndiotacticity of about 0.70.