This study aims to draw an exact boundary for microstructural and mechanical behaviors in terms of pulsed plasma nitriding conditions. The pulsed plasma nitriding treatment was applied to AISI 304 austenitic stainless steel at different temperatures and durations. Results reveal that nitriding depth increased as process temperature and duration increase. The nitriding depth remarkably increased at 475°C for 8 h and at 550°C for 4 h. An austenite structure was transformed into a metastable nitrogen-oversaturated body-centered tetragonal expanded austenite (S-phase) during low-temperature plasma nitriding. The S-phase was converted to CrN precipitation at 475°C for 8 h and at 550°C for 4 h. Surface hardness and fatigue limit increased through plasma nitriding regardless of process conditions. The best surface hardness and fatigue limit were obtained at 550°C for 4 h because of the occurrence of CrN precipitation.