Preparations, crystal structures, and spectral and magnetic properties of two new chiral one-dimensional cyano-bridged coordination polymers, [(CuL2)-L-II][M-II(CN)(4)]center dot 2H(2)O (M-II = Ni-II (1) and Pt-II (2), L = trans-cyclohexane-(1R, 2R)-diamine) have been presented. Complex 1 crystallizes in the monoclinic P2(1) space group with a = 9.864(4) angstrom, b = 15.393(8) angstrom, c = 7.995(4) angstrom, beta = 110.32(3)degrees, V = 1138.4(10)angstrom(3), and Z = 2, while 2 crystallizes in the monoclinic P2(1) space group with a = 9.899(3) angstrom, b = 15.541(4) angstrom, c = 8.102(2)angstrom, beta = 111.02(2)degrees, V = 1163.6(5)angstrom(3), and Z = 2. The unique zigzag cyano-bridged chains along the crystallographic b axis consist of alternate chiral [CuL2](2+) cations and square-planar [M(CN)(4)](2-) anions. One side of the axial Cu-N(equivalent to C) bond distances are 2.324(6) and 2.34(1) angstrom with Cu-N equivalent to C angles of 137.8(6)degrees and 138.2(9)degrees for 1 and 2, respectively. On the other hand, the opposite side of the axial Cu-N(equivalent to C) bond distances are 3.120(8) and 3.09(1) angstrom with significantly large bent Cu-N equivalent to C angles of 97.9(5)degrees and 96.8(7)degrees for 1 and 2, respectively. The novel axial bonding features of extremely long semi-coordination Cu-N bonds are attributed to coexistence of pseudo-Jahn-Teller elongation and electrostatic interaction in the unique zigzag cyano-bridged chains. The characteristic bonding features with overlap between small 3d (Ni-II) or large 5d (Pt-II) and 3d (Cu-II) orbitals results in larger shifts in XPS peaks of not only Cu2p(1/2) and Cu2p(3/2) but also Ni2p(1/2) and Ni2p(3/2) for 1 than those of 2, which is also consistent with weak antiferromagnetic interactions with Weiss constants of -5.31 and -5.94 K for 1 and 2, respectively. The d-d, pi-pi*, and CT bands in the electronic, CD, and MCD spectra for 1 and 2 in the solid state at room temperature are discussed from the viewpoint of magneto-optical properties.