The invention relates to a pH-responsive three-dimensional ordered macroporous controlled-release material. The sizes of macropores and communicating windows of the pH-responsive three-dimensional ordered macroporous controlled-release material are uniform, the sizes of the macropores are 100-1000nm, the sizes of the communicating windows are 40-120nm, and the pore volume is 1.3-2.8 cm<3> / g; the substrate is monodisperse three-dimensional ordered macroporous crosslinked polystyrene with windows which are mutually communicated, and a pH-responsive polymer chain section is introduced into the substrate by an atom transfer free-radical activity-controllable graft polymerization method; and the uncurling-curling action of the pH-responsive polymer chain section under different pH values is utilized to control the opening and closing of the communicating windows among the macropores: as the pH value increases, macromolecule chains gradually uncurl, and the pore windows are gradually closed, thereby realizing the controllable release of the contained filler. The pH-responsive three-dimensional ordered macroporous controlled-release material has wide application values in the controlled-release fields of biomedicine, medicine controlled-release systems, organized enzymes, slow release-embedding of catalysts, and the like.