Carbon-based composite materials are provided, such as those comprising at least 80 weight % of graphitic carbon comprising functional groups capable of forming hydrogen bonds, the graphitic carbon in the form of a mat of randomly entangled elongated structures; not more than 20 weight % of a polymer or a nanofiber thereof, dispersed within the graphitic carbon, the polymer or the nanofiber thereof comprising corresponding functional groups capable of forming hydrogen bonds with the functional groups of the graphitic carbon; and a plurality of hydrogen bonds at an interface formed between the graphitic carbon and the polymer or the nanofiber thereof, the plurality of hydrogen bonds formed between the functional groups of the graphitic carbon and the corresponding functional groups of the polymer or the nanofiber thereof.