A method for preparing carbon nanoparticles (CNPs) with controllable hierarchic structures is developed by combining the precursor-defined pyrolysis and the template method. Well-organized monodisperse CNPs, such as spherical particles with 3D porous structures (a), hollow carbon orbs containing small Pt particles (b), and graphitic microbeads with or without slits (c), are prepared by using structurally different precursors (see figure).