We demonstrate a simple and cost-effective technique, namely, one-photon absorption based direct laser writing (DLW), for direct fabrication of desired polymeric structures containing gold nanoparticles (Au NPs) and investigate their nonlinear optical properties. By focusing a continuous-wave laser at 532 nm with only a few milliwatts on a hybrid metal complex/photoresist material, we achieve an optically assisted local thermal effect, which results in the direct creation of Au NPs inside a polymerized SU-8 resist. The Au NP size is in the range of 10−50 nm, and the density is about 100 NPs per polymerized SU-8 resist voxel. By movement of the focusing laser beam, various polymeric structures containing Au NPs are patterned on demand, with the smallest feature size of about 500 nm. Furthermore, because of the nonlinear properties of the as-formed Au NPs, the hybrid structure exhibits a strong secondharmonic generation (SHG) signal when excited by a pulsed infrared laser. We then explore the application of Au NPs doped polymeric structures for nonlinear optical imaging. It is demonstrated that SHG is strong thanks to the plasmonic effect of individual Au NPs and their coupling, which strongly enhances the fundamental light intensity.