Using two types of triol ligands, several novel asymmetrically triol-functionalized Anderson organic hybrids have been efficieritly synthesized in high purity and good yields via a convenient two-step esterification reaction. These Organic inorganic hybrids are Chiral and can be spontaneously resolved with suitable solvents. Their molecular and crystal structures have been confirmed by single-crystal X-ray diffraction studies. Stable solid-state chirality of the corresponding enantiopure crystals has also been confirmed definitively by CD spectra. Interestingly, these organic inorganic hybrids possess a layer-by-layer structure, forming solvent-accessible nanoscale chiral channels via a 1D infinite helical chain substructure. TGA measurements indicated that the species of the central heteroatoms significantly effects the stability of these compounds.