Abstract 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 pomegranate‐like Fe 3 O 4 @N–C NCs possess a high specific capacity (1204.3 mA h g −1 at 0.5 A g −1 over 100 cycles), a stable cycle life (1063.0 mA h g −1 at 1 A g −1 , 98.4% retention after 1000 cycles), and excellent rate capacities (606.0 mA h g −1 at 10 A g −1 , 92.0% retention; 417.1 mA h g −1 at 20 A g −1 , 91.7% retention after 1000 cycles).