The reduction in the friction coefficient and minimizing wear are fundamental characteristics of friction components. Sulfurization effectively enhances the self-lubricating properties of metallic surfaces, while nitriding/carburizing can enhance the resistance to wear. This study explored two methods to create a sulfonitrocarburizing layer on 38CrMoAl. One method involved a simultaneous treatment of ammonia, carbon dioxide, and hydrogen sulfide, while the other employed a two-step process of initial nitrocarburizing, polishing, and sulfurization. The single-step treatment resulted in erratic COF and poor wear resistance. In contrast, the two-step treatment produced a composite structure of FeS polycrystals, sulfur-containing nanocrystals, and a nitrocarburizing layer. Further optimization made the composited structure achieve equilibrium between self-lubrication and binding force, resulting in a significant friction reduction effect exceeding 800 s and good occlusion resistance. This study presents a paradigm for successfully integrating treatments for strengthening metal surfaces, demonstrating the potential to enhance the efficacy of friction components.