AbstractFe2O3 nanoparticles (<10 nm) anchored on carbon nanotubes (denoted as Fe2O3‐NPs@CNT) are synthesized by a facile electrophoretic deposition strategy. In the composite, CNTs are utilized to construct a conductive matrix for uniformly dispersing Fe2O3‐NPs, building up a hierarchically porous architecture. The Fe2O3‐NPs anchored on CNTs can function as active sites for electrochemical reactions and facilitate fast electrochemical reaction kinetics, endowing the composite with improved electrochemical reversibility and desirable lithium storage capacity. The CNT framework can tightly hold Fe2O3‐NPs and thus provides fast electron transport to Fe2O3‐NPs, favouring high power performance in lithium‐ion batteries. The hierarchically porous structure can buffer the volume expansion/contraction caused by lithium insertion/extraction reactions. As expected, the composite delivers an ultrahigh reversible lithium storage capacity of 1231 mA h g−1 after 750 cycles at a high current rate of 1 A g−1. After tolerating the repeated volume fluctuation in the long cycle test, the composite still maintains its nanoporous architecture.