Abstract Chlorpyrifos as one of organophosphorus pesticides, is easily absorbed by human skin and dangerously causing inhibition of acetylcholinesterase that is essentially required for transporting nerve impulse. Therefore, the current approach focused on the adsorptive removal of Chlorpyrifos using superior adsorptive membrane composed of Al-metal organic framework@cellulose acetate (MIL-53-NH2@CA). The membrane was uniquely synthesized in two sequential steps; firstly, preparation of porous CA membrane and consequently, incorporation of MIL-53-NH2 within the synthesized porous CA membrane. Procedure was performed to impregnate various ratios of MIL-53-NH2 (20–60%) within the porous CA membrane. Micro-particles MIL-53-NH2 was successively immobilized within the membrane, while, the pore diameter was ranged in 124.5–485.6 nm. Adsorptive removal of chlorpyrifos through the prepared membrane was corresponded to Langmuir isotherm and pseudo-second ordered reaction. The maximum adsorptive capacity was observably increased from 160.36 mg/g for CA to 207.62–356.34 mg/g for MIL-53-NH2@CA. Impregnation of 60% MIL-53-NH2 resulted in fastening of the adsorptive removal rate of chlorpyrifos by factor of 2.2. The employed membrane exhibited very good recoverability and the adsorptive compatibility was diminished by 27.9% after five reuses. The prepared MIL-53-NH2@CA membrane can be promisingly applicable in the superior removal of pesticides and in various environmental applications.