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MoC/MoO 2 nano dots (QDs) heterostructure and defect engineering can promote each other to deliver electrons to the carbon substrate. Eventually, driven by the electronic modulation of multi-interface, MoC/MoO 2 -NCF can effectively accelerate the overall reaction kinetics. [Display omitted] The design and fabrication of advanced counter electrodes (CEs) for dye-sensitized solar cells (DSSCs) are limited by the scarcity of active sites and poor durability. Herein, we report the controlled preparation of a heterostructured nanoreactor CE based on defect-rich N -doped carbon nanoflowers (NCF) encapsulating MoC/MoO 2 nano dots (NDs) in a well-defined heterophase (MoC/MoO 2 -NCF). The MoC/MoO 2 NDs were uniformly dispersed on the NCF, and the NCF limited the size of the MoC/MoO 2 NDs and prevented their agglomeration, thus maximizing the electrochemically active surface area of MoC/MoO 2. Moreover, the synergistic effect between the MoC/MoO 2 interface and the N -defects is conducive to the full exposure of the active sites. Furthermore, theoretical calculations revealed that the MoC/MoO 2 heterojunction played a unique role in modulating the electronic structure and regulating the adsorption energy of tri-iodide in the iodide reduction reaction. The MoC/MoO 2 -NCF CEs in DSSCs demonstrated a power conversion efficiency (PCE) of 9.92% and high durability, exceeding the PCE (8.36%) and durability of Pt CEs. Overall, this study offers insights into the controlled synthesis of high-performance Mo-based composite CE materials for DSSCs. [ABSTRACT FROM AUTHOR]