Precursor-controlled thermolysis has been developed to specifically prepare structured carbonaceous materials (see figure) by using simple, but structurally defined, organic-cobalt complexes as starting compounds. The carbon-metal nanocomposites show excellent lithium storage properties as an anode material in lithium-ion batteries after controllable oxidation. They may also be useful as catalysts for fuel cells and other heterocatalytic reactions and as sensors for detecting chemicals and biomaterials.