In the present study, a novel Zr-pillared montmorillonite(Zr-MMT) macroporous materials (P-ZMt) was developed by dry pressing molding combining with pore forming agent. The structure and morphologies of P-ZMt was characterized by X-ray diffraction(XRD), scanning electron microscope(SEM), the thermal properties of samples were studied by thermal gravimetric analysis (TG), and the porosity of P-ZMt was detected by mercury porosimetry analyzer. The influence of porosity, permeability coefficient and specific surface area(SSA) including the mass ratio of different pore forming agent, pore forming agent dosage, pressure on of P-ZMt were evaluated. The adsorption of Cu2+, Cr3+, Pb2+, Cr6+ on P-ZMt was discussed. The optimum conditions for forming P-ZMt were: m(PMMA):m(AC)= 1:2, w(pore forming agent)=40%, pressure and calcination temperature were 20MPa and 550C, respectively. The pore size of P-ZMt varied from around 150μm to 250μm and the porosity up to 39.85%. The macropore of P-ZMt were interpenetration and the hole wall rendering three-dimensional honeycomb pore. When the adsorbent dosage was 1g/L, the removal rates of P-ZMt for Cr3+, Cu2+, Pb2+ were over 90%, while for Cr6+ almost no adsorption.