We report an anhydrous, autogenic technique for synthesizing electronically interconnected, carbon-encapsulated, nanoparticulate anatase anode materials (TiO2–C) for lithium-ion batteries. The TiO2–C nanoparticles provide a reversible capacity of ∼200mAhg−1, which exceeds the theoretical capacity of the commercially attractive spinel anode, Li4Ti5O12 (175mAhg−1) and is competitive with the capacity reported for other TiO2 products. The processing method is extremely versatile and has implications for preparing, in a single step, a wide variety of electrochemically active compounds that are coated, in situ, with carbon.