To produce a three-dimensional micro/nanocarbon structure, a manufacturing design technique for sub-10 nm carbon fiber arrays on three-dimensional carbon micropillars has been developed; the method involves initiating electrostatic jetting, forming submicron-to-nanoscale PAN-based fibers, and maximizing the shrinkage from polyacrylonitrile (PAN)-based fibers to carbon fibers. Nanoforming and nanodepositing methods for polyacrylonitrile-based jet fibers as precursors of carbon fibers are proposed for the processing design of electrostatic jet initiation and for the forming design of submicron-to-nanoscale PAN-based fibers by establishing and analyzing mathematical models that include the diameter and tensile stress values of jet fibers and the electric field intensity values on the surfaces of carbon micropillars. In accordance with these methods, an array of jet fibers with diameters of ~80 nm is experimentally formed based on the thinning of the electrospinning fluid on top of a dispensing needle, the poking of drum into an electrospinning droplet, and the controlling of the needle–drum distance. When converting thin PAN-based jet fibers to carbon fibers, a pyrolysis method consisting of the suspension of jet nanofibers between carbon micropillars, the bond between the fibers and the surface of the carbon micropillar, and the control of micropillar spacing, stabilization temperature, and carbonation rate is presented to maximize the shrinkage from PAN-based fibers to carbon fibers and to form sub-10 nm carbon fiber arrays between three-dimensional carbon micropillars. The manufacturing design of a three-dimensional micro/nanocarbon structure can produce thin PAN-based jet nanofibers and nanofiber arrays aligned on micropillar surfaces, obtain shrinkage levels reaching 96% and incorporate sub-10 nm carbon fibers into three-dimensional carbon micropillars; these actions provide new research opportunities for correlated three-dimensional micro/nanocarbon structures that have not previously been technically possible.