Three forms of modified coal-based adsorbents were developed and characterized as potential enhanced structurers during the removal of acephate pesticide. The raw coal (CA) was oxidized by nitric acid, forming nitrogen functionalized coal (N.CA), and both CA and N.CA were hybridized with polyaniline polymers (PANI/CA and PANI/N.CA). The adsorption performances of the modified structures in comparison with CA were evaluated based on both the steric and energetic parameters of the applied advanced isotherm model (the monolayer model of one energy). The uptake performances reflected higher capacities for the PANI hybridized form (261.9 mg/g (PANI/CA) and 316.6 mg/g (PANI/N.CA) as compared to N.CA (232.3 mg/g) and raw coal (201.2 mg/g). This signifies the impact of nitrogen functionalization and PANI hybridization on the surface properties of coal. The steric investigation determined the saturation of the coal surface with extra active sites after the nitric acid treatment (Nm (N.CA) = 103.5 mg/g) and the PANI hybridization (Nm (PANI/CA) = 119.07 mg/g and Nm (PANI/N.CA) = 146.4 mg/g) as compared to raw coal (Nm (CA) = 81.9 mg/g). This illustrated the reported uptake efficiencies of the modified samples, which can be attributed to the enhancement in the surface area (5.4 m2/g (CA), 18.3 m2/g (N.CA), 27.7 m2/g (PANI/CA), and 36.2 m2/g (PANI/N.CA)) and the incorporation of additional chemical groups (NO, C-N, and N-H). The results also reflect that each site can be loaded with three molecules of acephate, which are arranged vertically and adsorbed by multi-molecular mechanisms. The energetic studies (<40 kJ/mol) suggested the physical uptake of pesticide molecules by dipole bonding and hydrogen bonding processes. The thermodynamic functions reflect the exothermic properties of reactions that occur spontaneously.