The invention discloses a preparation process of a green environmentally-friendly high-adsorption-active adsorbent for printing and dyeing wastewater. The process comprises the following steps: mixingfly ash, bentonite and concentrated sulfuric acid, stirring, filtering, washing, drying, adding beta-type hemihydrate gypsum, manganese oxide and iron oxide, and uniformly mixing to obtain a fly ashcomposite; mixing carbon nanotubes and spherical alumina, stirring uniformly, adding an ethanol solution, stirring, adding microcrystalline cellulose, stirring, and washing to obtain a carbon nanotubecomposite; mixing sodium hexametaphosphate and water uniformly, adding the fly ash composite and the carbon nanotube composite, uniformly mixing, sending into a mold, drying in an oven, demolding, sending a molded blank body into a muffle furnace for roasting, and cooling to obtain the green environmentally-friendly high-adsorption-active adsorbent for the printing and dyeing wastewater. The preparation process is basically non-polluting, green and environmentally friendly, a product is not easy to loose in the adsorption process, the adsorption activity is high, adsorbed materials not only includes dyes in the printing and dyeing wastewater, but also includes some metal ions, the adsorption effect is better, and the problem of decolorization of the printing and dyeing wastewater is solved.