Recently, adopting carbon coating has drawn considerable attention for increasing the electrical conductivity and enhancing the stability of the electrode materials as elastic buffer supports upon cycling to improve the electrochemical performance. [27][28][29][30][31] Even through the volume changes may be effectively controlled by flexible substrates, this strategy is still limi ted in improving specific capacity and rate performance. Nanoengineering of ultrafine nanostructure (ultrafine nanoparticles or ultrafine nanosized subunits) has become the most powerful mean to tackle above challenge because they can increase the electrodeelectrolyte contact area, lower the absolute volume change, and shorten the distance for lithium-ion diffusion within the particles. [32,33] For instance, 3D mesoporous Co 3 O 4 networks composed of small Co 3 O 4 nanoparticles (5-10 nm) synthesized by Naiqin Zhao exhibit high specific capacity (1033 mA h g −1 at 0.1 A g −1 ) and remarkable rate capability. [34] Furthermore, robust and favorable ultrafine secondary nanoparticles would effectively accommodate the severe volume variation upon cycling and prevent self-aggregation of the ultrafine nanoscale subunits, thus leading to improved capacity retention and rate capability. For example, polydopamine-coated SnO 2 nanocrystals comprising SnO 2 nanoparticles (diameter ≈ 5 nm) developed by Lin and co-workers display excellent rate capability. [35] Nevertheless, the existing synthetic methods can only fabricate the ultrafine nanoparticles with exposed or mosaic structure which have disadvantages of inevitable aggregation and unstable nanostructure during long-term cycling; moreover, they are unsuitable for large-scale production. Hence, it is a great challenge to design and synthesize ultrafine carbon coating TMO subunit through a facile and one-pot method on a large scale.Along these lines, we develop a facile and novel one-pot approach for the first time to synthesize a series of highly uniform pomegranate-like TMO@nitrogen-doped carbon nanoclusters (TMO@N-C NCs) with a large scale production, which are organized by numerous of ultrafine TMO@N-C subunits (diameter ≈ 4 nm). This approach has been demonstrated to synthesize various pomegranate-like TMO@N-C NCs, including simple oxides such as Fe 3 O 4 , Mn 3 O 4 , NiO, and ZnO. Taking pomegranate-like Fe 3 O 4 @N-C NCs as an example, the pomegranate-like Fe 3 O 4 @N-C NCs with this unique nanostructure show excellent cycle stability and superior rate capacity Uniform pomegranate-like nanoclusters (NCs) organized by ultrafine transition metal oxide@nitrogen-doped carbon (TMO@N-C) subunits (diameter ≈ 4 nm) are prepared on a large scale for the first time through a facile, novel, and one-pot approach. Taking pomegranate-like Fe 3 O 4 @N-C NCs as an example, this unique structure provides short Li + /electron diffusion pathways for electrochemical reactions, structural stability during cycling, and high electrical conductivity, leading to superior electrochemical performance. The resulting...