In this study, we developed a simple surface-enhanced Raman Scattering (SERS) composite substrate, which is composed of an all-metal metasurface and on-surface random distributing silver nanoparticles (AgNPs), to enhance the performance of SERS sensing. The metasurface is made up of gold (Au) nanopillars array on aluminum (Al) and can localize the electromagnetic field energy with a resonant absorption peak near the 630 nm wavelength which contributes to the SERS performance of AgNPs deposited into the structure. The composite substrate can significantly improve the sensing performance, and the SERS Enhancement Factor (EF) reaches 2.81×106. The substrate also has good stability and reproducibility. The research is based on the combination of Localized Surface Plasmon Resonance (LSPR) and SERS effects, providing a method and idea for improving the sensitivity of SERS detection, and achieves the trace detection of Rhodamine 6G (R6G) and Thiram at 10-10 M, respectively.