Increasingly strict legislation for controlling the atmospheric emission of industrial volatile organic compounds (VOCs), which contribute to photochemical smog, ground-level ozone, and toxic air emissions, [1][2][3][4] has made the catalytic combustion of hydrocarbons a vital topic of research for the development of new processes for limiting air pollution by VOCs.[5] Oxides of transition metals such as Mn, Cr, Cu, and Co are the most commonly used, cost-effective catalysts for complete oxidation of VOCs, [6][7][8][9] and crystalline chromium oxide, which favors the formation of CO 2 , is the most promising candidate for the total oxidation of organics. [10] Ordered mesostructures of transition-metal oxides [11,12] are of immense interest in areas such as catalysis, sorption, chemical and biological separation, photonic and electronic devices, and drug delivery, [13] and well-ordered mesoporous oxides of Mn, [14] Ti, [15,16] V, [17] Zr, [18] W, [15] Nb, [15,17] and Ta [15,18] have been reported. However, the preparation of threedimensionally (3D) ordered mesoporous oxides of Cu, Co, Cr, Ni, and Fe is more difficult, although it has been possible to prepare unstable lamellar phases of these materials. Recently, hexagonally ordered mesoporous nickel oxide [19] and wormhole-like mesoporous iron oxide [20] have been reported. However, nanoporous 3D structure of oxides are more suitable for application as catalysts or adsorbents as they do not suffer from mass-transfer limitations and therefore allow the easier diffusion of reactants.[21] Transitional-metal oxides are more susceptible to hydrolysis, redox reactions, or phase transitions and possess a number of different coordination numbers and oxidation states, which makes it rather difficult to prepare mesoporous structures from them, unlike silica and aluminosilicates, which can easily form stable mesoporous structures. A neutral templating route has been successfully used for the synthesis of metal-oxide mesostructures [11,15] that are less readily accessible by electrostatic-templating pathways. [12,16] Herein we demonstrate for the first time that a 3D mesoporous chromium oxide material, prepared by a neutral templating route, shows an exceptionally high removal/ oxidation ability for VOCs (toluene, acetaldehyde) after calcination. For transition-metal oxides, control of the rates of precursor hydrolysis, condensation of metal species, and precipitation of mesostructured oxides, for example by slow crystallization, is an important prerequisite for the enhanced framework cross-linking [22,23] that leads to a stable mesoporous structure. We therefore used a metal nitrate salt precursor, a mixed nonaqueous, ethylene glycol/propanol medium, and poly(alkylene oxide) block copolymers as template to prepare a very stable 3D mesoporous structure. The mixed nonaqueous medium allows a very slow crystallization (gelation) process, which favors the formation of a stable mesostructure by enhanced framework cross-linking.