A novel 3,8-diimidazol-1,10-phen (phen = phenanthroline) compound has been prepared from the carbon-nitrogen bond cross-coupling reaction. X-ray structural studies for this compound and its dihydrate reveal they have different molecular conformations (L-b in 1 and L-c center dot 21-120 in 2). Two cadmium(II) and one zinc(II) complexes of 3,8-diimidazol-1, 10-phen, formulated as [Cd-2(D-caM)(2)(L,)(2)] center dot (H2O)(6) (3), [Cd-2(D-caM)(2)(L-a)(H2O)] (4), and [Zn-2(D-cam)(2)(Lb)(2)] center dot (H2O)(5) (5), have been obtained involving an auxiliary chiral ligand D-cam (a dianion Of D-camphoric acid) where the 3,8-diimidazol-1,10-phen ligand shows different molecular conformations, coordination modes, and architectures. Furthermore, D-cam and 3,8-diimidazol-1,10-phen ligands exhibit different bridging fashions to construct a homochiral 2D coordination polymer 3 and two homochiral 3D coordination polymers 4 and 5. Density function theory computational studies on comparing the different molecular conformations of the 3,8-diimidazol-1,10-phen ligand as well as spectral, nonlinear optical, and thermal properties for related compounds before and after the metal-ion complexation have also been carried out.