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In order to optimize the bifunctional electrocatalytic performance of La0.95FeO3-δ, the effects and influencing mechanism of carbon morphology, electrode ink preparation, and catalyst loading on the bifunctional electrocatalytic performance of oxygen reduction reaction (ORR) and oxygen evolution reaction (OER) were investigated. The results show that compared with La0.95FeO3-δ, the catalytic activity of La0.95FeO3-δ/C is significantly improved. The bifunctional electrocatalytic performance of La0.95FeO3-δ/C is mainly dependent on carbon morphology and electrode ink preparation. An optimum bifunctional performance is achieved in a composite electrode with 0.6 mg/cm2 La0.95FeO3-δ and 0.12 mg/cm2 EC600JD prepared by ultrasonic dispersion, ball milling, and ultrasonic dispersion. The optimized La0.95FeO3-δ/C has an excellent bifunctional electrocatalytic performance, simple preparation, and low cost, which is expected to be applied in Li-O2 batteries.