Abstract Uranium and uranium–zirconium electrodeposits produced in the Fuel Cycle Facility at Argonne National Laboratory-West were examined using standard metallurgical techniques. Substantial differences in the morphologies of the two types of deposits were observed. Samples from pure uranium deposits were comprised of chains of uranium crystals with a characteristic rhomboidal shape, while the morphologies of samples from deposits containing zirconium in excess of approximately 0.5 wt% showed more polycrystalline features. Zirconium was found to be present as a second, zirconium metal phase at or very near the uranium–zirconium dendrite surfaces. Higher collection efficiencies and total deposit weights were observed for the uranium–zirconium deposits; this performance increase is likely a result of better mechanical properties exhibited by the uranium–zirconium dendrite morphology.