The invention belongs to the technical field of adsorption materials, and particularly relates to an attapulgite and aniline-o-aminophenol composite adsorbent and a preparation method thereof. The preparation method comprises: S1, pretreatment: grinding attapulgite to obtain powder; S2, acidification: adding the powder to ultrapure water, stirring, standing, sucking the supernatant, taking the middle layer refined soil to obtain purified attapulgite, adding the purified attapulgite to a hydrochloric acid solution, vibrating, carrying out centrifugation, carrying out suction filtration on the suspension to obtain filter residue, and washing to achieve a neutral state so as to obtain acidified attapulgite; S3, modification: dissolving a coupling agent in an ethanol aqueous solution, dispersing, hydrolyzing, adding the acidified attapulgite, carrying out stirring filtering, washing, and drying to obtain modified attapulgite; and S4, in-situ polymerization: dissolving aniline and hydrochloric acid in ultrapure water, adding o-aminophenol and the modified attapulgite slurry, uniformly mixing, adding ammonium persulfate, carrying out suction filtration after completing the reaction, washing the obtained filter residue until the filtrate is colorless, drying the filter residue, and grinding. According to the present invention, the adsorbent can effectively adsorb Cr(VI) in wastewater.