<p>Improving the oxygen evolution reaction (OER) performance or replacing OER with the value-added conversion of biomass is of great significance for the green hydrogen energy production. In this work, bimetallic species-decorated laser-induced graphene (LIG) was fabricated and demonstrated as the self-supported electrodes towards efficient OER and 5-hydroxymethylfurfural oxidation reaction (HMFOR). Three-dimensional LIG was obtained via one-step irradiation process under ambient conditions, and active metal species were then introduced through electrodeposition, with Ni-based catalyst as the primary catalytic material and Fe and Co as modified metals. Among, LIG-NiFe electrode achieved an extremely low overpotential of 241.7&#xa0;mV at a current density of 20&#xa0;mA/cm² for OER and demonstrated long-term stability. This could be attributed to the promoted formation of Ni³⁺ active centers by Fe modified and the intrinsic porous structure of LIG providing an enhanced surface area. As for LIG-NiCo, due to the low onset potential of Co for HMF, it could achieve 99.6% HMF conversion and yielded value-added 2, 5-furandicarboxylic acid (FDCA) with a selectivity of 87.1%. Coupled with the merit of facile fabrication of LIG framework, this study demonstrates that LIG-based electrodes assume great practical application value in electrocatalytic reactions.</p> Graphical abstract <p></p>