Abstract: Vermiculite@starch carbide composites were prepared by hydrothermal carbonization of vermiculite and starch. The prepared composites were washed alternately with deionized water and absolute ethanol. The results of scanning electron microscopy (SEM) and infrared spectroscopy (FTIR) showed that starch carbide was successfully loaded on the surface of vermiculite. The preparation process of the composite was optimized by single factor and response surface method based on the phenol adsorbability index of the composite, and the optimal preparation process parameters were obtained as follows: The mass ratio of starch to vermiculite was 2.97∶1, the carbonization time was 15.66 h, and the carbonization temperature was 196.47 ℃. At these conditions, the composite material has the best adsorption performance for phenol, and its adsorption capacity for phenol is 16.521 mg/g, which is 4.304 mg/g higher than that of natural vermiculite.