Dual technique design in this research has successfully enriched the complementation between doping and surface modification. Here, Co(2+) doped Ag-ZnO nanocomposites (CAZ NCs) are mass produced by the combustion method. The HRTEM image shows that the doped Co(2+) and the surface modified Ag nanoparticles on the ZnO NCs are influential on the preferential orientation. Based on the conductivity formula σ = nqμ and the actual verification, the improved photoelectric properties of CAZ NCs under visible light irradiation are attributed to the enhanced light absorption and the weakened recombination of photogenerated electron-hole pairs. It would be instructive for the sound design concept of subsequent material development.