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The interface between metal oxide and conductive carbon material is important for rate performance and cycling stability of the electrode materials for lithium-ion batteries. Herein, we present a simple strategy for tightly anchoring ultra-small NiO nanoparticles on nitrogen-doped flower-like carbon scaffold through strong Ni–O–C and Ni–C dual chemical bonds. Benefiting from the robust interfacial interaction and high surface compatibility, the overall conductivity and structural robustness of the NiO/Ni/nitrogen-doped carbon complex improve significantly. Moreover, the unique open-porous structure which consists of interconnected carbon sheets provides sufficient electron/ion transport paths. Therefore, the composite reveals high capacity as high as 1025 mAh g−1 at 0.1 A g−1, superior rate capability (468 mAh g−1 at 2 A g−1) and remarkable cyclic stability (662 mAh g−1 retention after 500 cycles at 0.5 A g−1).