Novel graphene oxide-ordered mesoporous silica materials with two-dimensional mesoporous structure and large surface area were successfully fabricated through sol-gel and self-assembly methods. The synthesized materials were characterized by small-angle X-ray diffraction, scanning electron microscopy, transmission electron microscopy, and nitrogen adsorption-desorption. By taking advantage of the excellent properties, the hybrid materials were employed as the adsorbent for removal of heavy metals in environmental waters by adsorption separation-inductively coupled plasma mass spectrometry. The results showed that the materials exhibited superior adsorption capacity, the removal efficiencies for As, Cd, Cr, Hg, and Pb reached 97.7, 96.9, 96.0, 98.5, and 78.7 %, respectively. The facile, low-cost, and environmental friendly synthesis method as well as highly efficient adsorption ability made it become a promising adsorbents for the removal of toxic heavy metals at low or trace concentrations from wastewater.