The thermolysis of copper ferrimalonate Cu3[Fe(CH2C2O4)3]2⋅9H2O has been investigated up to 1073 K in flowing air atmosphere employing various physico-chemical techniques, i.e., simultaneous TG-DTG-DSC, XRD, Mössbauer, IR, and TEM. The precursor undergoes dehydration and decomposition simultaneously to yield copper malonate and iron(II) malonate intermediates at 433 K. At higher temperature (548 K) these intermediate species decompose to CuO and α-Fe2O3, respectively. Finally, copper ferrite, CuFe2O4, has been obtained as a result of solid state reaction between α-Fe2O3 and CuO at a temperature (623 K) much lower than that for conventional ceramic method. The TEM analysis of the final thermolysis product reveals the formation of monodisperse copper ferrite nanoparticles with an average particle size of 33 nm. Magnetic studies show that these nanoparticles exhibit saturation magnetization of 2783 G and Curie temperature of 709 K. Lower magnitude of these parameters as compared with the bulk values may be attributed to the ultrafine grain size of the ferrite particles.