In this study, the functional adsorbent metal-organic framework ZIF-8/magnetic multi-walled carbon nanotubes (M-M-ZIF-8) was successfully prepared for removal of eight organophosphorus pesticides from environmental water and soil samples. The M-M-ZIF-8 was characterized and their adsorption capacity was evaluated based on their isothermal adsorption curves. The results suggest that ZIF-8 particles are deposited on the surface of the magnetic MWCNTs via coordination-polymerization strategy. In addition, M-M-ZIF-8 has high static adsorption capacities for organophosphorus pesticides because of its high specific surface area and porous structure. The static adsorption data fit the Freundlich adsorption model better than the Langmuir model. Under the optimized conditions, M-M-ZIF-8 was successfully applied to remove the eight organophosphorus pesticides from environmental water and soil samples. A possible mechanism is valence-electron-driven adsorption by sharing or exchanging of electrons between the organophosphorus pesticide molecules and the vacant active sites of M-M-ZIF-8. Therefore, M-M-ZIF-8 is a promising hybrid adsorbent for adsorption and removal of organic pollutions from the environment.