We report a new adsorbent nanocomposite material based on matrix-dispersed superparamagnetic iron oxide nanoparticles (SPIONs) in molecularly-imprinted polyaniline for the removal of chlorpyrifos (CPF), a hazardous organophosphate pesticide, from water. The synthesized magnetic molecularly-imprinted polymer (MMIP) was characterized by FTIR spectroscopy, XRD, magnetic susceptibility, DLS, zeta potential measurement, SEM and high-resolution TEM imaging. The average size of the naked SPIONs ranges from 15 to 30 nm according to the high-resolution TEM analysis. Moreover, the adsorption kinetics, thermodynamic parameters (ΔG, ΔH and ΔS), adsorption isotherms and rebinding conditions were investigated in detail. The proposed MMIP has an imprinting factor of 1.64. In addition, it showed a high experimental adsorption capacity of 1.77 mg g⁻¹ and a removal efficiency of nearly 80%. The fabricated MMIP material demonstrated excellent magnetic susceptibility allowing for easy separation using an external magnetic field. The adsorption mechanism of CPF onto the MMIP adsorbent followed the second-order kinetics model and fitted to the Temkin adsorption isotherm. By studying the adsorption thermodynamics, negative ΔG values (−1.955 kJ mol⁻¹ at room temperature) were obtained revealing that the adsorption process is spontaneous. Furthermore, the maximum adsorption capacity was obtained at room temperature (ca. 303 K), neutral pH and using a high CPF concentration.