Despite having a low electrical conductivity, graphene oxide (GO) is used as an anode material in lithium-ion batteries (LIBs) owing its good processability in large quantities. GO is reduced by chemical or thermal treatments to enhance its electrical conductivity. In this study, high-performance GO anodes with polydopamine (PDA) and polyethylenimine (PEI) as binders were fabricated. Gamma (γ)-ray irradiation was applied to the GO–PDA–PEI hybrid sheets to covalently cross-link the GO sheets and binders with an amide bond. The covalent crosslinking was confirmed by Fourier-transform infrared spectroscopy analysis. Further, X-ray photoelectron spectroscopy results showed that γ-ray irradiation produced a reduced GO sheet, which resulted in an increase in the electrical conductivity by 30%. By characterizing the electrochemical properties, we found that the γ-ray irradiation facilitates the stability and increases the charge/discharge capacity by crosslinking GO and PDA–PEI binders and reducing the GO sheets.