Due to their outstanding power density, long cycle life and low cost, supercapacitors have gained much interest. As for supercapacitor electrodes, molybdenum nitrides show promising potential. Molybdenum nitrides, however, are mainly prepared as nanopowders via a chemical route and require binders for the manufacture of electrodes. Such electrodes can impair the performance of supercapacitors. Herein, binder-free chromium (Cr)-doped molybdenum nitride (Mo<inf>2</inf>N) TFEs having different Cr concentrations are prepared via a reactive co-sputtering technique. The Cr-doped Mo<inf>2</inf>N films prepared have a cubic phase structure of γ-Mo<inf>2</inf>N with a minor shift in the (111) plane. While un-doped Mo<inf>2</inf>N films exhibit a spherical morphology, Cr-doped Mo<inf>2</inf>N films demonstrate a clear pyramid-like surface morphology. The developed Cr-doped Mo<inf>2</inf>N films contain 0–7.9 at.% of Cr in Mo<inf>2</inf>N lattice. A supercapacitor using a Cr-doped Mo<inf>2</inf>N electrode having the highest concentration of Cr reveals maximum areal capacity of 2780 mC/cm2, which is much higher than that of an un-doped Mo<inf>2</inf>N electrode (110 mC/cm2). Furthermore, the Cr-doped Mo<inf>2</inf>N electrode demonstrates excellent cycling stability, achieving ~ 94.6% capacity retention for about 2000 cycles. The reactive co-sputtering proves to be a suitable technique for fabrication of binder-free TFEs for high-performance energy storage device applications. Graphical Abstract: [Figure not available: see fulltext.] © 2022 Elsevier B.V., All rights reserved.