In this study, the laser-induced graphitization process of sustainable chitosan-based formulations was investigated. In particular, optimal lasing conditions were investigated alongside the effect of borax concentration in the chitosan matrix. In all cases, it was found that the obtained formulations were graphitizable with a CO2 laser. This process gave rise to the formation of high surface area, porous, and electrically conductive laser-induced graphene (LIG) structures. It was found that borax, as a cross-linker of chitosan, enabled the graphitization process when its content was ≥30 wt % in the chitosan matrix, allowing the formation of an LIG phase with a significant content of graphite-like structures. The graphitization process was investigated by thermogravimetric analysis (TGA), Raman, X-ray photoemission (XPS), and Fourier transform infrared (FTIR) spectroscopies. LIG electrodes obtained from CS/40B formulations displayed a sheet resistance as low as 110 Ω/sq. Electrochemical characterization was performed after a 10 min electrode activation by cycling in 1 M KCl. A heterogeneous electron transfer rate, k0, of 4 × 10-3 cm s-1 was determined, indicating rapid electron transfer rates at the electrode surface. These results show promise for the introduction of a new class of sustainable composites for LIG electrochemical sensing platforms.