Nano-crystalline LiNi0.5Mn1.5O4 with a unique powder characterization has been successfully synthesized by a soft combustion reaction method, using lithium nitrate, manganese nitrate, and nickel nitrate as the starting materials, and no organic materials being introduced in the whole process. The LiNi0.5Mn1.5O4 powders synthesized by the soft combustion reaction method were investigated by differential thermal analysis and thermogravimetry, X-ray diffractometer, and transmission electron microscopy. The resultant product was a pure phase of LiNi0.5Mn1.5O4 without any other impurities. Electrochemical measurements were also performed.