Metal nanoparticle is of great importance for the study of surface plasmon resonance, and its functional assembly can show more excellent overall collaborative performance. We propose an efficient assembly of gold nanoparticles (GNP) through femtosecond laser fabrication without introducing additional modifier, which can not only retains the particle’s surface plasma resonance characteristic, but also realizes the assembling pattern of arbitrary subtle shape. We apply the assembly in microfluidic chip for surface-enhanced Raman scattering detection and achieve a very good enhancement. It provides a new approach for the preparation of plasma devices.