An electrodeposited crystalline functional chromium deposit which is nanogranular as deposited, and the deposit may be both TEM and XRD crystalline or may be TEM crystalline and XRD amorphous. In various embodiments, the deposit includes one or any combination of two or more of an alloy of chromium, carbon, nitrogen, oxygen and sulfur; a {111} preferred orientation; an average crystal grain cross-sectional area of less than about 500 nm2; and a lattice parameter of 2.8895+/−0.0025 A. A process and an electrodeposition bath for electrodepositing the nanogranular crystalline functional chromium deposit on a substrate, including providing the electrodeposition bath including trivalent chromium, a source of divalent sulfur, a carboxylic acid, a source of nitrogen and being substantially free of hexavalent chromium; immersing a substrate in the bath; and applying an electrical current to electrodeposit the deposit on the substrate.