Carbon aerogels are nanostructured carbons obtained from the carbonization of organic aerogels, which are prepared from the sol–gel polycondensation of certain organic monomers. These materials have a great versatility both at the nanoscopic level in terms of their pore texture and at the macroscopic level in terms of their form. Thus, the surface area, pore volume, and pore size distribution are tuneable surface properties related to the synthesis and processing conditions, which can produce a wide spectrum of materials with unique properties. In addition, carbon aerogels can be obtained in the form of monoliths, beads, powders or thin films. All these properties make them promising materials for application in adsorption and catalysis. Metal-doped monolithic organic aerogels can be easily prepared by following three main strategies: by addition of the metal precursor to the initial mixture, by ion-exchange or by deposition of the metal precursor on the organic or the carbon aerogel by one of various methods. These metal-doped carbon aerogels have been used as catalysts and as electrodes for electrical double-layer capacitors. This article shows the preparation of metal-doped carbon aerogels, their physico-chemical surface properties and their applications as catalysts in various reactions.