A thermally stable cadmium-based chiral metal-organic framework (MOF), {[Cd-2(L)(H2O)-(DMF)]center dot 3DMF center dot 2H(2)O}(n) (1; DMF = N,N-dimethylformamide), has been synthesized from an achiral ligand by spontaneous resolution. The MOF features 1D open channels with a large density of active metal sites and has a 3,6-c binodal net with a rare sit 3,6-conn topology. The metal-bound water and DMF solvents could be easily removed along with the guest molecules in the lattice upon activation to afford the desolvated framework 1'. It exhibits microporous nature, as confirmed by the gas-sorption measurements with carbon dioxide uptake of 43.2 cm(3) g(-1) at 273 K. The open metal sites in the framework make it an outstanding heterogeneous catalyst in the Strecker reaction for the synthesis of alpha-aminonitriles in a solvent free state at room temperature with excellent conversion yields.