Two new coordination polymers (CPs), [InCl(H2bidc)2(H2O)]n (1) and [Sc(Hbidc)(OH)(H2O)]n (2) (H3bidc = benzimidazole-5,6-dicarboxylic acid) were synthesized through a solvothermal approach. 1 exhibits a 1D infinite chain, which further constructs a 3D supramolecular framework via hydrogen bonds. 2 features a 3D supramolecular framework consisting of left- and right-handed chiral layers, which contain the left- and right-handed chiral spiral chains. The adjacent layers stack through π–π stacking interactions between benzene and imidazole rings. 1 exhibits excellent catalytic reactivity for the Strecker reaction and can be recycled four consecutive reactions with more than 95% conversion yields.