A batch study is conducted to remove methylene blue (MB) dye from an aqueous solution using coconut coir and its acid-treated forms. The sulfuric acid-treated coconut coir (SCC), phosphoric acid-treated coconut coir (PCC) and untreated coconut coir (UCC) were prepared. Adsorbents were characterized via BET, SEM, pHPZC, FTIR, and FT-Raman analysis. Adsorbent’s total organic carbon (TOC) and the number of oxygen-containing functional groups like carboxylic, lactonic and phenolic, total acidic, and basic groups were also estimated. FTIR and FT-Raman studies establish functional groups responsible for dye removal. The operating parameters were optimized through experiments. Dye was removed maximally at the lowest temperature, 303K. Langmuir and Temkin isotherm models use linear equations, and the Pseudo-second-order kinetic model uses a nonlinear equation, which fits well. The adsorption capacity of SCC, PCC and UCC adsorbents was 88.18 ± 0.63 mg/g, 92.68 ± 2.74 mg/g and 76.39 ± 0.36 mg/g, respectively, for 303K. Intraparticle diffusion dominated more than film diffusion. Physisorption was estimated by applying the Dubinin-Radushkevich (D-R) isotherm model. Thermodynamic study indicates a spontaneous, favorable, exothermic process. 75% glacial acetic acid and 100% methanol are the best solvents for desorbing dye-loaded adsorbents. Porous coir and non-covalent interactions like hydrogen bonding, van der Waals force and π-π interaction between dye and coir are vital in the dye removal process. The regression equation has been successfully formulated, and the application of a genetic algorithm has predicted the percentage removal of methylene blue dye.