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• By adding PVP and DMF to the precursor, lamellar LaFeO 3 material was successfully prepared. • Lamellar LaFeO 3 has smaller particle size and larger specific surface area. • The maximum discharge capacity of lamellar LaFeO 3 is up to high 372.1 mA h g–1 at the discharge current density of 60 mA g–1. • After 100 cycles, the specific discharge capacity of the lamellar LaFeO 3 can still reach 293.1 mA h g–1, which is much higher than that of 98.5 mA h g–1 for LaFeO 3. Compared with traditional hydrogen storage alloys, perovskite oxide LaFeO 3 materials are considered as one of the most promising anode materials for nickel-metal hydride batteries owing to their low cost, environmental friendliness, and superior temperature resistance. However, the biggest problem faced by perovskite oxide LaFeO 3 as an anode material for Nickel/metal hydride (Ni-MH) batteries is the low electrical conductivity and poor specific capacity, which is mainly due to the serious agglomeration phenomenon in its structure. To solve the above problems, lamellar LaFeO 3 material with large specific surface area and small particle size has been synthesized by adding N,N-Dimethylformamide (DMF) and polyvinyl pyrrolidone (PVP) inhibitor materials to the precursor. By changing the sintering temperature, the lamellar composite LaFeO 3 material can be controlled. Consequently, the maximum discharge capacity of lamellar LaFeO 3 is up to 372.1 mA h g–1 at the discharge current density of 60 mA g–1. Meanwhile, after 100 cycles, the specific discharge capacity of the lamellar LaFeO 3 can still reach 293.1 mA h g–1, which is much higher than that of 98.5 mA h g–1 for LaFeO 3. In addition, the kinetics of LaFeO 3 has been investigated and the lamellar LaFeO 3 shows excellent dynamic properties. Notably, the exchange current density I 0 (300 mA g–1) of the layered LaFeO 3 electrode is higher than that of LaFeO 3 (150 mA g–1). Overall, this work provides insights into a structure-performance relationship for the further development of high-performance perovskite-type oxide nickel-metal hydride battery anodes. Lamellar LaFeO 3 material with large specific surface area and small particle size has been synthesized by adding N,N-Dimethylformamide and Polyvinyl pyrrolidone inhibitor materials to the precursor. By changing the sintering temperature, the layered composite LaFeO 3 material can be controlled. Consequently, the maximum discharge capacity of lamellar LaFeO 3 is up to high 372.1 mA h g–1 at the discharge current density of 60 mA g–1. Meanwhile, after 100 cycles, the specific discharge capacity of the lamellar LaFeO 3 can still reach 293.1 mA h g–1, which is much higher than that of 98.5 mA h g–1 for LaFeO 3. [Display omitted] [ABSTRACT FROM AUTHOR]