Molybdenum is nitrided by a 100-Hz pulsed DC glow discharge technique for various time durations and fill gas pressures to study the effects on the surface properties of molybdenum. X-ray diffractometry (XRD), scanning electron microscopy (SEM), and atomic force microscopy (AFM) are used for the structural and morphological analysis of the nitrided layers. Vickers' microhardness tester is utilized to investigate surface microhardness. Phase analysis shows the formation of more molybdenum nitride molecules for longer nitriding durations at fill gas pressures of 2 mbar and 3 mbar (1 bar = 10 5 Pa). A considerable increase in surface microhardness (approximately by a factor of 2) is observed for longer duration (10 h) and 2-mbar pressure. Longer duration (10 h) and 2-mbar fill gas pressure favors the formation of homogeneous, smooth, hard layers by the incorporation of more nitrogen.