A nanocomposite of well-dispersed iron oxide nanoparticles (NPs) anchored on crumpled nitrogen-doped MXene nanosheets (N–Ti3C2/Fe2O3) is synthesized by solventless thermal decomposition of a precursor of iron-oleate complex mixed with N-doped MXene nanosheets (N–Ti3C2). In this hybrid structure, well-dispersed iron oxide nanoparticles anchored on the highly conductive N-doped MXene nanosheets can surely enable better electrons transfer and buffer the large volume change of the active material. Furthermore, they act as mutual spacers in the nanocomposite to effectively prevent the aggregation of the nanoparticles and the restacking of the MXene nanosheets. When used as anode for Li-ion batteries (LIBs), crumpled N–Ti3C2/Fe2O3 nanocomposites exhibit high reversible capacity (1065 mA h g−1 at 100 mA g−1), fast charge/discharge ability and robust cycling performance (remains at 549 mA h g−1 after 400 cycles at 2 A g−1), which suggesting this novel anode material has potential prospect for Li-ion batteries.