Mo4+ partially substituted spinel Li4Ti5-xMoxO12 (x=0.5-1.5) have been synthesized by the Pechini method. For a high substitution level such as x=1.5, single-phase product is difficult to prepare by this technique. At low annealing temperature, rutile is the secondary phase. At high annealing temperature, monoclinic Li4Mo5O12 appears as the secondary phase. Single-phase product can be readily made at lower substitution level. Mo4+ substitution of Ti4+ can increase electronic conductivity of the spinel, which improves the performance of the material in lithium-ion batteries and electrochemical capacitors. (c) 2007 The Electrochemical Society.