A novel, oleic acid-assisted solution combustion synthesis route has been successfully explored to synthesize high surface area and mesoporous Al-doped LiMn2O4 nanosheets without the use of MnO2 templates. The as-synthesized LiMn2O4 nanosheets possess the typical electrochemical superiorities. The high surface area of 44.5 m2g−1, high porosity, and layered structure have been desirable and perquisites for enhanced supercapacitor applications. These nanosheets present strong (400) planes than normal, easing the charge transfer during electrochemical processes. An enhanced specific capacitance of 433 Fg−1 is obtained along with the enhanced rate capabilities. The high energy and high power density of 23.4 Whkg−1 and 4651 Wkg−1 respectively make the LiMn2O4 nanosheets an effective cathode material in supercapacitor applications. The novel solution combustion method provides an effective single-step approach to synthesize desired LiMn2O4 nanostructures for enhanced next generation energy applications.