A new end-to-end thiocyanato-bridged 1D polymeric copper(II) complex [CuL 1 (l 1,3 -NCS)] n (1), and a new end-on azido-bridged dimeric copper(II) complex [CuBrL 2 (l 1,1 -N 3 )] 2 (2), where L 1 is the deprotonated form of 2-[1-(2-methylaminoethylimino)ethyl]phenol (HL 1 ) and L 2 is N-methyl-N 0 -(1-pyridin-2-ylethylidene)ethane-1,2-diamine, have been synthesized and structurally characterized by elemental analysis, IR spectra, and single-crystal X-ray diffraction. Complex 1 crystallizes in the monoclinic space group P2 1 /n with unit cell dimensions a = 10.822 (1) Å , b = 10.054(1) Å , c = 12.532(2) Å , b = 106.810 (2)°, V = 1305.3(3) Å 3 , Z = 4, R 1 = 0.0341 and wR 2 = 0.0766. Complex 2 crystallizes in the monoclinic space group P2 1 /n with unit cell dimensions a = 10.427(2) Å , b = 10.672(2) Å , c = 12.626(2) Å , b = 108.069(9)°, V = 1335.7(4) Å 3 , Z = 2, R 1 = 0.0346 and wR 2 = 0.0714. The Cu atom in 1 is in a square pyramidal coordination, and that in 2 is in an octahedral coordination. The CuÁÁÁCu distances are 6.406(1) Å in 1, and 3.762(1) Å in 2. The pseudohalide anions are versatile bridging groups for the construction of polymeric structures of Schiff base copper(II) complexes.