A chiral, nonracemic pentadentate pyridine bis(oxazoline) ligand forms unprecedented P-helical inorganic−organic hybrid polymers with cadmium halides. The one-dimensional chains consist of Λ2-configured pentagonal-bipyramidal cadmium complexes with metal-centered chirality bridged by [CdX4]2- tetrahedra via shared halide atoms. In the solid state, the overall helicity exhibits strongly directed orientation parallel to the crystallographic axis a.