Using a gangue as raw in the experiment, the process of synthesizing gangue-based adsorbent with high crystallinity and purity by self-transformation of gangue in vapor phase of ethylamine and water at a temperature range of 373 ~ 400 K was researched. The adsorption properties of the gangue-based adsorbent were studied by means of static nitrogen-adsorption capacity method so that the nitrogen-adsorption isotherm, specific surface and pore distribution were reached. Through the adsorbing experiment of phenol, the phenol- adsorption isotherm of the gangue-based adsorbent was obtained. The experiments indicated that the proper adsorbing temperature, large specific surface area and suitable membrane process were effective to enhance the adsorption capacity of the gangue-based adsorbent.