The as-cast, two-phase, f.c.c. + B2, lamellar-structured, high-entropy alloy Fe 28.2 Ni 18.8 Mn 32.9 Al 14.1 Cr 6 was annealed in pure nitrogen at either 800°C or 1000°C for 100 h in order to harden the surface by nitridation. Similar nitriding treatments were performed on a comparably-structured, four-component alloy Fe 30 Ni 20 Mn 35 Al 15 for comparison. Scanning electron microscopy and energy dispersive X-ray spectroscopy were used to analyze the resulting microstructures and phase compositions. AlN formation near the surface completely depleted the matrix of Al resulting in a f.c.c. matrix containing AlN particles, while a two-phase lamellae structure remained in the center of the specimens. Nevertheless, the AlN-containing region exhibited a higher hardness than the AlN-free area. Interestingly, the presence of Cr led to much more rapid diffusion of nitrogen into the material