Lithium copper pyrophosphate has been synthesized by the solution combustion method for the first time. Urea and hexamethylenetetramine were used as fuel. The samples were successfully prepared in low reaction temperature and short reaction time. The products were structurally characterized by FT-IR and p-XRD. Thermal behavior of samples was also investigated through TG/DT analyses. Magnetic measurements showed that the urea- and hexamethylenetetramine-assisted Li₂CuP₂O₇ were paramagnetic at room temperature. Surface analyses indicated that the fuel types changed the surface properties of samples because of exothermic redox reaction during combustion, and electrochemical performances showed clear differences. The charge capacity of urea- and hexamethylenetetramine-assisted synthesized Li₂CuP₂O₇ was calculated as 180 mAhg⁻¹ and 146 mAhg⁻¹. Synthesis method enlarged the charge capacity and prepared lithium copper pyrophosphate to have a potential for use in lithium-ion batteries.