The oxidation of alcohols to carbonyl compounds is an important reaction in synthetic organic chemistry. While stoichiometric oxidants are effective for this transformation, they often produce large amounts of toxic waste, which renders them unacceptable from an environmental and economic perspective. Consequently, there is a strong impetus to develop catalytic processes that utilize environmentally friendly, inexpensive primary oxidants, the use of molecular oxygen being particularly attractive. Recently, hydrotalcites have attracted attention as both catalysts and catalyst supports for the selective oxidation of alcohols to ketones and aldehydes, using either oxygen or TBHP as the oxidant. This review is intended to provide a comprehensive summary of work performed in this area to date. The effects of composition and structure on catalyst properties are highlighted, and mechanistic aspects are discussed.