The adsorption mechanism of dichlorvos onto coconut fibre biochar (CFB) was investigated by the batch adsorption technique. Coconut fibre waste material was synthesised at 600 °C for 4 h under oxygen-limited conditions. The biochar was modified by HCl acid to enhance the specific surface area and porosity. The characteristics of the biochar were analysed by scanning electron microscopy (SEM), Brunauer-Emmett-Teller (BET) specific surface area, and Fourier transform-infrared (FT-IR). The results showed that the BET specific surface area of biochar was 402.4 m2/g. Experimental data presented a good fit to Langmuir isotherm and the pseudo-second-order model. Langmuir isotherm illustrated that monolayer adsorption of dichlorvos occurred on the surface of CFB, with a maximum adsorption capacity of 90.9 mg/g. The diffusion model confirmed that the liquid film diffusion was the rate-limiting step, and the major diffusion mechanism of dichlorvos onto biochar. The BET result after dichlorvos adsorption demonstrated that pore-filling occurred and occupied 58.27%. The pore-filling and chemical interactions, performed important roles in the adsorption of dichlorvos onto CFB. Chemical adsorption is comprised of two interactions, which are hydrophobic and H-bonding, but the prime is H-bonding. CFB is a very potential material for the removal of dichlorvos and environmental pollutants.