A systematical study has been employed on 2D TiO2 nanosheets with the donor-acceptor codoping. The (2Nb/2Ta + C) codoping in TiO2 nanosheets creates the delocalized midgap states. The C-related systems are desirable visible and UV-light-driven photocatalysts. The water splitting power of (Mo/W + 2N) codoped systems is improved with enhanced UV light response. The high doping concentration means the stronger absorption ability of the solar energy.