Four helical semiconductor framework materials assembled from chalcogenide II-VI nanoclusters have been synthesized and characterized. These cadmium sulfide clusters form intertwined helical assemblies from helices of either the same handedness or the opposite handedness, resulting in the crystallization of cluster-decorated chiral quartz net and achiral moganite net. The UV-vis diffuse reflectance spectroscopy and the simultaneous TG-DSC analysis show that these helical materials are wide-gap semiconductors with band gap between 3.0 and 3.4 eV and are thermally stable up to about 300 degrees C.