trode materials for the replacement of the conventional graphite. [1][2][3][4][5][6] However, they suffer from a variety of problems such as poor conductivity for the oxides/ hydroxyls/sulfides and bad structural stability for the nitrides. [7][8][9][10][11] Some of the common methods used to solve the above problems include nanostructuring, [12] carbon coating, [13,14] mixing with carbonbased materials, [15,16] and the construction of TMC composites. [17,18] The preparation of TMC composites usually combines the advantages of each material, leading to synergistic effect. [19][20][21] According to the study by J. Maier, the phase interface present in a composite often leads to lattice mismatch and therefore creates more active sites for energy storage, enabling the electrodes to exceed their theoretical capacity. [22,23] Moreover, the lattice mismatch is also beneficial for the transformation of lithium ions and electrons, which could also result in the improved rate performance. On the other hand, the predominant pseudocapacitive processes in lithium-ion batteries make active materials show better rate capability. [24] Many electrode materials such as MoO 3 , [25] SnO, [26] and SnS [27] have been found with excellent pseudocapacitive characteristics both in lithium and sodiumion batteries because these materials store more energy at the surface or near surface of the material by Faradaic charge transfer. [1] Pseudocapacitance materials can either be intrinsic (i.e., storage properties not based on particle sizes and morphologies such as RuO 2 and MnO 2 ) or extrinsic (i.e., storage properties based on the preparation of porous or nanometersized active materials such as V 2 O 5 and MoO 2 ). [27] Moreover, pseudocapacitive contributions have been obtained in some insertion, conversion, and alloying reaction of individual or single electrode materials, while their application in composites has been less studied. [28] In view of advances of various TMC composite electrodes, it is highly challenging to study their relationship to pseudocapacitance contributions.Among the commonly reported electrode materials with pseudocapacitive properties, nickel-based materials (NiO, Ni 3 S 2 , and Ni 3 N) have attracted intense attention due to their low cost and theoretical capacity higher than that of conventional graphite. [29] Several strategies have been employed to improve the performance of energy storage devices through the development of new electrode materials. The construction of transition metal compound composite electrodes plays an important role in promoting the performance of energy storage devices. However, understandings of and insight into how to enhance the composites properties are rarely reported. Taking nickel-based compounds as an example, Ni 3 N@ Ni 3 S 2 hybrid nanosheets are reported as a high-performance anode material for lithium-ion batteries that delivers higher lithium storage properties than the pristine Ni 3 N and Ni 3 S 2 electrodes. This demonstrates that the phase boundaries between the Ni 3 N...