H2O2 plays a critical role in the electro-Fenton process for treating organic contaminants. Herein, recyclable binder-free unique 3D LaFeO3@TiO2-NTs/Ti cathodes are constructed to efficiently degrade tetracycline via in situ produced H2O2 using a facile electrochemical deposition method. H2O2 with a high production rate of 1.602 μmol cm–2 h–1 is generated to maximize reactive oxide species, and the degradation efficiency of tetracycline can reach 97.83% in 2 h with a low LaFeO3 loading density of 0.0793 mg cm–2. A radar chart is proposed to evaluate the contribution degree of condition factors for the tetracycline removal efficiency. LaFeO3@TiO2-NTs/Ti exhibits improved stability and recyclability, and the removal efficiency remains at 93.5% after 10 cycles. The tetracycline degradation mechanism and pathways are discussed. Recyclable 3D electrodes are promising for efficient pollution control via increasing the life and accessible active sites.