An electron beam (EB) was irradiated on carbon anodes of lithium-ion secondary batteries. The discharge capacity was increased by 19mAhg−1 in the mesocarbon microbeads electrode and by 55mAhg−1 in the coffee-bean derived carbon electrode. X-ray photoelectron spectroscopy (XPS) and Raman spectroscopy were used to observe the surface changes which included a reduction in the amount of binder and structural changes in the carbon materials.