An amphiphilic chitosan-loaded bentonite adsorbent (C18CTS−BT) was prepared for the efficient removal of organic matter from coking wastewater. The structure and surface morphology of adsorbents were characterized by FT−IR, XRD, and SEM. The removal of those organics by C18CTS−BT was investigated by comparing the adsorption performances of C18CTS−BT with bentonite (BT) and chitosan-loaded bentonite (CTS−BT). The results showed that compared with BT and CTS−BT, C18CTS−BT showed the performance advantages of having a low dosage, wide pH range, and short adsorption equilibrium time. The optimized treatment process was as follows: the adsorbent dosage was 1.5 g·L−1, the adsorption time was 60 min, and the pH of the system was 7.0. The chemical oxygen demand (COD) of the coking wastewater treated with BT, CTS−BT, and C18CTS−BT decreased from 342 mg·L−1 in the raw water to 264 mg·L−1, 218 mg·L−1, and 146 mg·L−1, corresponding to COD removal rates of 22.81%, 36.26%, and 57.31%, respectively. The results of GC−MS analysis also confirmed that C18CTS−BT could remove most of the organic compounds in coking wastewater, especially long−chain alkanes and their derivatives. The hydrophobic modification of the adsorbent material can effectively improve the removal performance of organic compounds from coking wastewater.