Gas-phase room-temperature methane activation by various clusters draws increasing attention. In this Letter, we produce a series of bimetallic oxide clusters which contain both main-group metal aluminum atoms and transition-metal vanadium atoms. We provide solid experimental and theoretical evidence that bimetallic AlVO4+ cluster can draw a hydrogen atom from methane to produce CH3 at room temperature. The Al3VO7+ cluster which can be considered as a system formed from Al2O3 + AlVO4+ does not break C-H bonds of methane. The results enrich the chemistry of gas phase methane activation and provide possible molecular level mechanism to couple with heterogeneous catalysis. (C) 2010 Elsevier B. V. All rights reserved.