Abstract: In an exemplary method, a nano-architectured carbon structure is fabricated by forming a unit (e.g., a film) of a liquid carbon-containing starting material. A surface of the unit is nano-molded using a durable mold (122) that is pre-formed with a pattern of nano-concavities corresponding to a desired pattern of nano-features to be formed by the mold on the surface of the unit. After nano-molding the surface of the unit, the first unit is stabilized to render the unit and its formed nano-structures capable of surviving downstream steps. The mold is removed from the first surface to form a nano-molded surface of a carbonization precursor (152). The precursor is carbonized in an inert-gas atmosphere at a suitable high temperature to form a corresponding nano-architectured carbon structure (62). A principal use of the nano-architectured carbon structure is a carbon electrode used in, e.g., Li-ion batteries, supercapacitors, and battery-supercapacitor hybrid devices.