The invention relates to preparation and application of a magnetic ferroferric oxide nanoparticle modified carbon nanotube composite material. The preparation method includes: mixing a divalent iron salt and a trivalent iron salt, adding NH3.H2O, conducting water bath and centrifugal separation, washing the precipitate, and carrying out drying and grinding to obtain magnetic Fe3O4 nanoparticles; adding concentrated nitric acid and concentrated sulfuric acid into pretreated carbon nanotubes, conducting heating refluxing, carrying out filtering, deionized water washing and vacuum drying, thus obtaining purified multiwalled carbon nanotubes; adding the purified multiwalled carbon nanotubes into a triethylene glycol solution, conducting ultrasonic treatment, adding magnetic Fe3O4 nanoparticles, performing stirring and heating, conducting heat preservation and cooling, separating the product, and conducting vacuum drying, thus obtaining the magnetic Fe3O4 nanoparticle modified carbon nanotube composite material. The composite material is used for detecting the residue amount of organophosphorus pesticides in food. The preparation method utilizes magnetic Fe3O4 nanoparticles to modify carbon nanotubes, and greatly improves the dispersibility and adsorption properties of carbon nanotubes in water. The prepared magnetic Fe3O4 nanoparticle modified carbon nanotube composite material hasgood stability, and the maximum recovery rate can reach 89.6%.