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Despite the excellent electrochemical performance of MnO-based electrodes, a large capacity increase cannot be avoided during long-life cycling, which makes it difficult to seek out appropriate cathode materials to match for commercial applications. In this work, a grape-like MnO−Ni@C framework from interfacial superassembly with remarkable electrochemical properties was fabricated as anode materials for lithium-ion batteries. Electrochemical analysis indicates that the introduction of Ni not only contributes to the excellent rate capability and high specific capacity but also prevents further oxidation of MnO to the higher valence states for ultrastable long-life cycling performance. Furthermore, thermodynamic calculation proves that the ultrastable long cycling life of the Ni−Mn−O system originated from a buffer composition region to stabilize the MnO structure. Because of the unique grape-like structure and performance of the Ni−Mn−O system, the MnO−Ni@C electrode displayed an invertible specific capacity of 706 mA h g −1 after 200 cycles at a current density of 0.1 A g −1 and excellent cycling stability maintained a capacity of 476.8 mA h g −1 after 2100 cycles at 1.0 A g −1 without obvious capacity change. This new nanocomposite material could offer a novel fabrication strategy and insight for MnO-based materials and other metal oxides as anodes for improved electrochemical performance.