Metal oxides (MOs) materials represent a promising route to address our nation’s energy challenges because of their widespread use in/or supports for highly efficient catalysts, gas separation/storage, and optoelectronic materials. We describe our multifaceted approach which includes synthesis, characterization (thermodynamic, modeling and neutron scattering) and modification of MgO and ZnO based materials. A novel vapor based method is used to produce pure and doped MgO and ZnO with narrow size distribution and selective microstructure. These MO materials can be produced in sizes ranging from a few to several hundred nanometers. Each of these two MO based sets of materials exhibit attractive physicochemical properties that can be employed in carbon capture/sequestration, as well as energy (hydrogen/methane) storage/conversion, and catalysis. Recently, our interests have been focused on decorating the MOs supports with small metallic clusters (e.g. Pd and Cu) or individual atoms using both chemical and physical vapor deposition methods. A few examples of our investigations using hydrogen and methane gas sorption will be presented to illustrate the power and promise of such an approach.