Black matter in catalysis: Graphitic carbon catalyzes the insertion of O atoms into acrolein. Such complex multistep atom rearrangements were believed to be the exclusive domain of metal (oxide) catalysis. In the C‐catalyzed process, the nucleophilic O atoms terminating the graphite (0001) surface abstract the formyl H atom and the activated aldehyde is oxidized by a mobile epoxide O atom. Thus, the sp2 carbon acts as a bifunctional catalyst.