Novel well-defined superparamagnetic Fe 3 O 4 @Bacilus subtilis composite (Fe 3 O 4 @B. subtilis SPMC) was synthesized through a facile electrostatic attraction method and used as a recyclable heterogeneous Fenton-like catalyst. With the presence of H 2 O 2 , Fe 3 O 4 @B. subtilis SPMC can remove nearly 87% of the doxycycline at the initial concentration of 50 mg L −1 , exhibiting enhanced Fenton-like catalytic performance than pristine Fe 3 O 4 . The mechanism study demonstrates the synergistic effect between Bacilus subtilis adsorption and Fenton-like ability of Fe 3 O 4 dominates the enhancement for Fenton-like catalytic efficiency of Fe 3 O 4 @B. subtilis SPMC. The obtained composite shows excellent recycling ability, reusability, and stability, which pave a new way for future design on highly efficient Fenton-like catalyst for degradation of organic pollutants.