The mesoporous ferrisilicates (MFS) with high iron content were synthesized by pH-modification method, and the iron content could be up to 10.5wt.% (Si/Fe=8). The pH was kept less than 2 at pre-hydrothermal synthesis step and was adjusted to 11 during hydrothermal step. The samples were characterized by XRD, HRTEM, N 2 -sorption, XRF, FTIR, DRUV–vis, Fe K-edge EXAFS, EPR, and DSC. The results suggested that the MFS materials were ordered 2D hexagonal mesophase of MCM-41, and the iron atoms were tetrahedral coordinated in the silica framework. This material could efficiently catalyze the hydroxylation of phenol in water medium using H 2 O 2 as an oxidant, and the phenol conversion could be up to 52% under the optimal experimental conditions.