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We report an efficient method to synthesize vertically aligned Co3O4nanostructures on the surface of cobalt foils. This synthesis is accomplished by simply heating the cobalt foils in the presence of oxygen gas. The resultant morphologies of the nanostructures can be tailored to be either one‐dimensional nanowires or two‐dimensional nanowalls by controlling the reactivity and the diffusion rate of the oxygen species during the growth process. A possible growth mechanism governing the formation of such nanostructures is discussed. The field‐emission properties of the as‐synthesized nanostructures are investigated in detail. The turn‐on field was determined to be 6.4 and 7.7 V μm–1for nanowires and nanowalls, respectively. The nanowire samples show superior field‐emission characteristics with a lower turn‐on field and higher current density because of their sharp tip geometry and high aspect ratio.