Surface functionalized mesoporous silicates, MCM-41s, having 3-(2-pyridylmethylideneimino)propyl group (PI-MCM-41) or 3-(2-quinolylmethylideneimino)propyl group (QI-MCM-41) were prepared via Schiff base reaction, and the adsorption behavior of metal ions onto the modified MCM-41s was investigated. The function groups on the modified MCM-41 surface were confirmed by Fourier transform infrared spectroscopy (FT-IR), X-ray photoelectron spectroscopy (XPS), and elemental analysis. The metal ions examined, Co2+, Ni2+, Cu2+, Zn2+, Cd2+, and Pb2+, were quantitatively adsorbed on the PI-MCM-41 and QI-MCM-41, except for Mn2+. In the complexation with these metal ions, it was suggested that imine-N and heterocyclic-N atoms act as donor atoms. In addition, it was considered that the hydrophobicity derived from the organo-functional groups modified on MCM-41 contributed to improving the adsorption ability.