In this work, we report a new type anode material, MoO2 combined carbon dots (CDs) with nanoparticle-stacking structure via a facile hydrothermal route. Herein, CDs is introduced as the reductant which in-situ reduces MoVI to MoIV. It is further confirmed that the particles of MoO2 with evenly distributed beset of carbon dots form a nanoparticle-stacking structure. Thanks to this specific structure, the as-made MoO2-CDs manifest high performance in lithium-ion batteries (LIBs) and sodium-ion batteries (SIBs). The capacities maintain 854 and 236 mAh g−1 at 0.50 A g−1 after 300 cycles for LIBs and 600 cycles for SIBs, respectively. Furthermore, we explored the structure-stability relationship by the electrochemical measurement and morphology, found the mechanisms of charge/discharge composed of dominant redox reaction and auxiliary intercalation reaction, and explained the characteristics of a high rate performance through kinetic issues and extrinsic pseudocapacitance contributions. This green synthetic method of anode material could make it possible to obtain high-performance alkali-ion batteries and other energy storage devices.