Two types of manganese oxides, the octahedral layer structure(OL) and the octahedral molecular tunnel structure(OMS), were controllably synthesized via a facilely hydrothermal route and used to remove heavy metal ions(Pb2+, Cu2+, Ni2+, Hg2+) in solutions. The heavy metal ion concentrations before and after adsorption were determined by atomic absorption spectroscopy (AAS) and atomic fluorescence spectroscopy (AFS) to evaluate the material adsorption performance. The competitive adsorption of the four ions (Pb2+, Cu2+, Ni2+, Hg2+) on manganese oxides was also investigated. The results showed that OMS exhibited better adsorption ability than OL and had excellent adsorption selectivity to Pb2+, with 98% adsorption efficiency in two minutes. Therefore, this can be proposed as a simple, green and efficient method for treatment of polluted water.