MoO2 nanocrystals (NCs) on Ni foam were simply synthesized via a facile hydrothermal method and a dip-coating method. It was worth noting that ultrafine interconnected MoO2 nanocrystals (about 10 nm) were uniformly anchored on Ni foam to fabricate a particular three-dimensional architecture, which may provide more active sites and shorter transmission pathways for lithium ions. As binder-free anode, MoO2 NCs on Ni foam deliver a high initial discharge capacity of 990 mAh·g-1 and retain a reversible capacity of 924 mAh· g-1 after 100 cycles at a current density of 0.1 C. More importantly, when the current density returns from 2 C to 0.1 C, the capacity recovers to 910 mAh·g-1 (about 92％ of the original high capacity), suggesting excel-lent cycling stability and rate capability. The particular 3D electrode as binder-free anode makes it a promising anode candidate for high-performance lithium-ion batteries.