A crystalline chromium deposit having a lattice parameter of 2.8895+/−0.0025 Å, and an article including the crystalline chromium deposit. An article including a crystalline chromium deposit, wherein the crystalline chromium deposit has a {111} preferred orientation. A process for electrodepositing a crystalline chromium deposit on a substrate, including providing an electroplating bath comprising trivalent chromium and a source of divalent sulfur, and substantially free of hexavalent chromium; immersing a substrate in the electroplating bath; and applying an electrical current to deposit a crystalline chromium deposit on the substrate, wherein the chromium deposit is crystalline as deposited.