This study represents a green synthesis method for fabricating an oxygen evolution reaction (OER) electrode by depositing two-dimensional CuFeOxon nickel foam (NF). Two-dimensional CuFeOxwas deposited on NF usingin situhydrothermal synthesis in the presence ofAloe veraextract. This phytochemical-assisted synthesis of CuFeOxresulted in a unique nano-rose-like morphology (petal diameter 30–70 nm), which significantly improved the electrochemical surface area of the electrode. The synthesized electrode was analyzed for its OER electrocatalytic activity and it was observed that using 75%Aloe veraextract in the phytochemical-assisted synthesis of CuFeOxresulted in improved OER electrocatalytic performance by attaining an overpotential of 310 mV for 50 mA cm−2and 410 mV for 100 mA cm−2. The electrode also sustained robust stability throughout the 50 h of chronopotentiometry studies under alkaline electrolyte conditions, demonstrating its potential as an efficient OER electrode material. This study highlights the promising use ofAloe veraextract as a green and cost-effective way to synthesize efficient OER electrode materials.