The invention relates to a metal-organic framework UiO-66 adsorbent and a modified material thereof. The adsorbent is prepared by a conventional solvothermal technology. A zirconium source and an organic ligand are mixed, and then are dissolved in a solvent, a solution obtained after the complete dissolving of the zirconium source and the organic ligand is added into a stainless steel reactor witha polytetrafluoroethylene liner, a substance formed after the reaction is washed with an organic solvent and then is filtered, and the obtained solid is dried to obtain the target adsorbent with thepore diameter of 1.4-2.0 nm and the specific surface area of 885-1500 m<2>/g. The modified adsorbent is prepared by a one-step technology by using P123 as a template or CTAB as a surface modifier, andthe obtained product contains the modified UiO-66 with a meso-porous structure or the UiO-66 adsorbent with a functional group. The above adsorbent materials have stable performances, and can be applied to the adsorption of toluene at 298-373 K and the adsorption of toluene in a high humidity atmosphere.