A series of nitrogen-doped coconut shell activated carbon catalysts were prepared by urea or melamine impregnation followed by heat treatment and used for the removal of methyl mercaptan (CH₃SH). The physical and chemical properties of the nitrogen-doped coconut shell activated carbons were evaluated by nitrogen adsorption/desorption, scanning electron microscopy, X-ray photoelectron spectroscopy, elemental analysis, Boehm titration, and thermal analysis. The results show that CH₃SH capacity depends on the nitrogen content. Further research indicates that pyridinic nitrogen and quaternary nitrogen are the active sites. Due to the metal-free property of the nitrogen-rich coconut shell activated carbon, the regeneration process can be easily performed and dimethyl disulfide (CH₃SSCH₃) can be recovered as the main product. Our study indicates that there is a promising prospect for nitrogen-rich coconut shell activated carbon for CH₃SH removal because of its high capacity, mild conditions, and easy regeneration.