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Summary: Strontium (Sr) incorporated LaMnO3 (La0.7Sr0.3MnO3) nanoparticles have been synthesized by ball‐milling‐assisted solid‐state reaction to study their performance as electrode material for energy storage applications. The La0.7Sr0.3MnO3 nanoparticles exhibit superior electrochemical performance in neutral aqueous electrolyte (1 M Na2SO4) in comparison to LaMnO3 and SrMnO3 nanoparticles. This neutral electrolyte provides relatively higher ionic conductivity and viscosity compared to the ionic liquids and a wider potential window compared to the alkaline electrolytes. Electrochemical study of the electrodes prepared using La0.7Sr0.3MnO3 nanoparticles reveals pseudocapacitive behaviors with fast reversible Faradaic charge storage, which plays a key role in charge storage. The composite materials exhibit highest specific capacitance of 393.5 F g−1 at a scan rate of 2 mV s−1. Asymmetric supercapacitors fabricated using La0.7Sr0.3MnO3 nanoparticle and activated carbon operates over a wide potential window of 1.8 V, and it reveals high specific capacitance (197 F g−1) as well as high capacitive retention (87%) even after 4000 charge–discharge cycles. [ABSTRACT FROM AUTHOR]