In this work, laser shock peening (LSP) was utilized as a surface-processing technique to modify the tribo-corrosion characteristics of cold-spray (CS) 316L SS. Results indicate that with the influence of LSP, the degree of wear-corrosion synergism was effectively decreased. Particularly, the degree of wear loss being accelerated by electrochemical degradation was effectively reduced due to the cumulative effects of refined crystallinity, increased surface hardness, closure of surface pores, and decrease in wettability. Consequentially, the wear mechanism transitioned from being an abrasive type with cracking and delamination to an abrasive type free of any defects. From these findings, it can be inferred that LSP is indeed a viable method to improve the tribo-corrosion characteristics of CS 316L SS.