Chiral compounds are successfully photosynthesized by coupling redox biocatalysis with the photoregeneration of nicotinamide cofactors on quantum-dot-sensitized TiO2 nanotubes under visible light irradiation. Nanotubular morphology and hybridization of TiO2 with CdS enables highly efficient photoregeneration of cofactors by ensuring better diffusion of reaction species and rapid charge separation.