The synthesis of nanostructured carbon materials with a highly ordered graphitic structure is of great interest because of their unique physico-chemical properties, including high electrical conductivity and chemical stability for multipurpose applications in current industries. [1-3] The current synthetic process for a highly ordered graphitic structure from carbonaceous materials requires an energy intensive process, including heating at extremely high temperatures (>2000 °C). [4,5] Furthermore, most amorphous carbon and organic molecules are classified into nongraphitizable carbon precursors, whereas only a few precursors, which can be organized into a grain with a local molecular orientation (LMO), form a highly ordered graphitic structure. [6,7] Therefore, the formation of highly ordered graphitic structures derived from non-graphitizable precursors using readily available synthetic methods has been a challenge. Recently, metal-catalyst-assisted graphitization has been attempted to prepare graphitic carbon structures through heat treatment at relatively low temperatures. [8-12] It was recently found out that the hollow carbon shells can be obtained by the direct thermal conversion of a Ni-based metal organic framework (MOF) at 1000 °C. [13] Xia et al. reported that a graphitic carbon nanocage was synthesized by the spray pyrolysis of iron carbonyl at 900 °C. [14] Although it was claimed that the carbon nanocage has well-developed graphitic layers along with a unique microstructure, the resulting materials only exhibited short-range order, thereby hindering the genuine role of functional graphite. Unlike previous approaches, Bin et al. prepared nanostructured graphite by heating Ketjen black to 2800 °C, which imparted additional functionalities to graphite. [15] Temperatures higher than 2000 °C are believed to be essential to realize graphitization from several graphitizable precursors. [4,5] This paper introduces a novel and sustainable method to synthesize 3D graphite nanoballs (GNBs) by the low-temperature pyrolysis of a non-graphitizable precursor, tannic acid (TA). This is the first report of metal-phenolic coordination compounds with which low-temperature graphitization can be done in one-pot synthesis. Abundant phenol groups on the TA molecules tend to bond with atomically distributed Ni-ions via a metal-phenolic coordination reaction. [16-19] The Ni 2+-TA Continuous efforts have been made to achieve nanostructured carbon materials with highly ordered graphitic structures using facile synthetic methods. 3D graphite nanoballs (GNBs) are synthesized by the lowtemperature pyrolysis of a non-graphitizable precursor, tannic acid (TA). Abundant phenol groups on TA bind to Ni 2+ to form metal-phenolic coordination, which renders each Ni cation to be atomically distributed by the TA ligands. Even at low temperatures (1000 °C), highly ordered graphitic structure is promoted by the distributed Ni nanoparticles that act as a graphitization catalyzer. The crystallinity of the GNB is fully corroborated by the inten...

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