Honeycomb-like structured graphitic carbon nitride (g-C3N4 ) with tunable band structure was prepared through a one-step salt-template assisted approach. The honeycomb structure, cyano group defects and Na ion doping result in enhanced light absorption, improved photoexcited charge carrier separation, and up-shift of conduction band. As a consequence, the photocatalytic H-2 evolution rate is about 5.2 times higher than that of the pristine graphitic carbon nitride. This newly developed approach provides a promising way to modify other functional materials through nanostructure design coupled with electronic modulation strategy simultaneously.