The ferroferric oxide @ silicon pillared montmorillonite catalytic material (Fe3O4@SPC) was prepared by a one-step interlayer template method using calcium-based montmorillonite (Ca-MMT).The morphology and structure of the material were characterized by XRD, FTIR, BET and SEM. The results showed that Fe3O4@SPC has d001=3.30 nm large crystal plane spacing and 4.47 nm mesoporous aperture, and most of Fe3O4 particles were dispersed on the surface of SPC. The catalytic activity and stability of Fe3O4@SPC were evaluate with phenol. The optimized conditions were as follows: the mass concentration of phenol is 100 mg/L, the pH value is 3.5, the mass concentration of catalyst is 0.5 g/L, H2O2 dosage of 0.2 mL and the reaction time is 120 min, the degradation rate of phenol is 100%. The removal rate of phenol remained above 90% after the catalyst was recycled for 5 times. Tert-butyl alcohol quenching experiment, revealed that ?OH oxidation played a key role in heterogeneous Fenton-like catalytic oxidation degradation of phenol. And the possible degradation path of phenol was speculated by the intermediates of phenol degradation with GC-MS.