The efficient removal of Tetracycline Hydrochloride (TC) from wastewater, which is a difficult process, has attracted increasing attention. Aiming to synchronously achieve the goal of natural waste utilization and PMS activation, we have combined the MOFs material with waste coffee grounds (CG). The catalytic activity of the CG@ZIF-67 composite in the TC removal process was thoroughly evaluated, demonstrating that the TC removal rate could reach 96.3% within 30 min at CG@ZIF-67 composite dosage of 100 mg/L, PMS concertation of 1.0 mM, unadjusted pH 6.2, and contact temperate of 293.15 K. The 1O2 and ·SO4- in the CG@ZIF-67/PMS/TC system would play the crucial role in the TC degradation process, with 1O2 acting as the primary ROS. The oxygen-containing functional groups and graphite N on the surface of CG@ZIF-67 composite would play a major role in efficiently activating PMS and correspondingly degrading TC. In addition, the CG@ZIF-67/PMS/TC system could withstand a wide pH range (3â11). The application of CG in preparing MOF-based composites will provide a new method of removing emerging pollutants from an aqueous solution.