A facile and effective method to fabricate highly pseudocapacitive electrodes of Fe–Ti–O@C has been proposed here. In this strategy, FeOOH crystals were firstly grown uniformly on the surface of Ti-based MOF (MIL-125) tablet substrates through a solution immersion method, and then converted to uniform carbon supported Fe–Ti–O composites by calcination under argon. The obtained Fe–Ti–O@C composites were first utilized as an efficient anode for lithium ion batteries with a high reversible capacity of 988 mA h g⁻¹ after 160 cycles at 200 mA g⁻¹. Such a superior lithium storage performance may be due to the synergistic effect of the Fe₃O₄ nanoparticles with a high capacity, FeTiO₃ nanocomposites with a nearly stable structure during the Li⁺ insertion/removal process, and the conductive carbon skeleton with a large surface area and porous structure. This work represents an important step forward in the fabrication of MOF-derived hybrids and enables transition metal oxides (TMOs) to have potential applications in energy storage systems.