A new neodymium-phosphine compound (Nd-(Ph)3P) was used for the first time as an electrode for supercapacitors and exhibited an extraordinary capacitance of 951 F g-1 at 0.5 A g-1 with a high capacitance retention of 96% after 10 000 cycles at 10 A g-1, which is the highest capacitance for rare earth based materials in SCs. Such an excellent performance might be due to the fact that this material can provide plenty of electron-active sites for charge storage and electrolyte diffusion can be efficiently promoted.