Moreover, the abundant nanovoids on the sp 2 -hybridized carbon shell and interior space of CNOs facilitate the loading of pseudocapacitive species (metal oxides, [11] the conductive polymer, [12] functional groups, [13,14] etc.) and corresponding charge transport during the charge-storage process. Although fascinating performance has been achieved by CNOs, the efficient synthesis of CNOs remains a great challenge, seriously impeding its application in supercapacitors.Great efforts have been made on the synthesis of CNOs in the past decades. Series of synthetic techniques such as chemical vapor deposition (CVD), [15] underwater electric arc discharge, [16] carbon ion implantation, [17] and annealing of nanodiamonds [18] have been developed to achieve CNOs with tunable sizes (5-200 nm), shapes (spherical and polyhedral), and types of cores (hollow and dense). Among various techniques, chemical methods including CVD, the thermal transformation of nanodiamonds, and thermal pyrolysis of carbon precursor were considered as more viable methods for the production of CNOs, especially in large-scale (gram quantities). For instance, Chen et al. [19] reported a gramscale CVD synthesis of hollow CNOs with MgO supported Co as the catalyst. The hollow CNOs consist of defective carbon shells with diameters ranging from 10 to 50 nm. Recently, the functionalized onion-like graphitic carbon nanospheres (5-30 nm in diameter) were fabricated by a high-temperature transformation of nanodiamonds at 2700 °C, providing the high surface area with multiple oxygen functional groups for enhanced Li-ion storage. [20] Nevertheless, these techniques still suffer from the use of large contents of catalyst (>50 wt%) and high temperature (>1700 °C) [21] in the gram-scale synthesis of CNOs.Herein, we demonstrate a novel bubble template for efficient assembly of CNOs at gram-scale, by using sticky pitch to coat on petroleum coke. The corresponding formation mechanism was proposed and the key feature of this approach is the confinement of petroleum coke generated gas bubbles (H 2 ) to serve as the pristine fragments of graphitic shells for the assembly of CNOs. The as-synthesized CNOs present a uniform particle size of ≈5-30 nm, a superior surface area up to 2665.5 m 2 g −1 , and a large pore volume of 1.2 cm 3 g −1 , which favor the ionic diffusion as well as electronic transport in supercapacitors. Significantly, the CNOs electrode delivered a high specific capacitance of 312 F g −1 at 1 A g −1 and retained as high Carbon nano-onions (CNOs), recognized as multilayered fullerenes, display superior electrical conductivity (comparable with carbon black) and large surface area due to the highly defective sp 2 carbon shells, making it a promising member of carbon nanomaterials for energy applications. However, the lack of efficient synthesis of CNOs in large-scale production (gram quantities) has impeded their range of commercial applications. Herein, for the first time, it is demonstrated that the gram-scale synthesis of CNOs is developed by simply an...