This study reports the usage of chemically impregnated coconut coir waste (CICCW) as a low-cost adsorbent for the desulfurization of feed diesel. The characterization of the developed adsorbent was focused on quantitative analysis (carbon yield %, proximate, ultimate, carbon surface functionalities, BET surface area and porosity distribution, and particle size analysis), qualitative analysis (FTIR), and optical analysis (SEM). Batch experiments with feed diesel having a total sulfur concentration of 2,050 mg L−1 were conducted to optimize the adsorption parameters such as adsorbent dose, temperature, and contact time. The adsorption process shows an optimum dose of 1 g/20 mL, and the equilibrium is attained in 3 h. The adsorption of sulfur onto the adsorbent at optimum temperature 293 K is regulated by external mass transfer (diffusion into mesopores) followed by a steady adsorption phase with intra-particle diffusion in micropores. A Fickian mechanism controls the diffusion of sulfur molecules from the solution onto the surface of the adsorbent. Freundlich adsorption isotherm illustrates the equilibrium adsorption data very well. The negative value of ΔG° (−27.61 kJ mol−1) and ΔS° (−44.56 J K−1 mol−1) indicates the feasibility, spontaneity of the adsorption process and justified the decrease in the randomness of adsorbed sulfur molecules onto the adsorbent surface, respectively. The exhausted CICCW can be effectively regenerated by methanol and reutilized for three adsorption–desorption cycles. The approximate cost of preparation of the adsorbent was USD 10.714 per kg. These results clearly proved the feasibility of the developed low-cost adsorbent (CICCW) as a good candidate for the desulfurization of feed diesel.