In this work, a novel and efficient Fe-Ni LDH@ZIF-67 catalyst modified carbon cloth (CC) cathode was developed for tetracycline (TC) degradation in heterogeneous electro-Fenton (Hetero-EF) process. Compared to Fe-Ni LDH/CC (75.7%), TC degradation rate of Fe-Ni LDH@ZIF-67/CC cathode increased to 95.6% within 60 min. The synergistic effect of hetero-EF and anodic oxidation process accelerated electron transfer, the maximum HO production of Fe-Ni LDH@ZIF-67/CC electrode reached 264 mg/L, improving utilization efficiency of HO. The cathode possessing a satisfied TC degradation performance over a wide pH (3-9). Free radical capture experiment revealed the collaboration of ·O, ·OH, and O play a significant role in TC degradation. The 5 cycles experiment and metal ion leaching experiment showed that the proposed Fe-Ni LDH@ZIF-67/CC has good recyclability and stability. In addition, the proposed Fe-Ni LDH@ZIF-67/CC cathode achieved satisfying performance in real water (tap water: 97.3%, lake water: 97.7%), demonstrating the possibility for practical application. TC degradation pathways were proposed by theory analysis and experimental results. The toxicity of TC intermediates was reduced by Hetero-EF degradation according to Toxicity Estimation Software Tool and Escherichia coli growth inhibition experiments. This work provides a novel modified cathode to improve removal efficiency of antibiotics in wastewater.