wo rare-earth zirconate oxides RE2Zr2O7 (RE = La and Nd) with pyrochlore structures were fabricated, employing a simple and modified solid-state route. After confirmation of their microstructure, physicochemical features, and morphologies, the fabricated pyrochlores were applied for electrochemical hydrogen storage, and their capacity was compared in an alkaline medium. The La2Zr2O7 microstructure exhibited an enhanced electrochemical hydrogen storage performance (maximum discharge capacity = 2350 mAh/g) compared to the Nd2Zr2O7 structures. Having a higher specific surface, as well as a more favorable physical and chemical nature, could be responsible for this more suitable performance. Lanthanum zirconate ceramic microstructure could be introduced as an active material with an appropriate capacity for electrochemical hydrogen storage.