A one-step process to fabricate crystalline Li4Ti5O12(LTO) particles directly from solution using an atmospheric pressure plasma jet (APPJ) is reported. This process uses Ti and Li ions-containing salt solutions as the precursor, which is ultrasonically nebulized and then transported to the downstream of the APPJ using a carrier gas. With an extremely short contact time (<0.1 s) between the precursor droplets and the plasma jet, crystalline LTO can be fabricated in one step without additional rinse and postannealing steps. The LTO particle size can be effectively controlled using a preheater, the precursor solution composition and concentration, and the carrier gas flow rate. By properly adjusting the operating condition, particles of diameters from 100 nm to few μm with various morphologies can be obtained. When used as an electrode material, the resulting LTO powders fabricated under selected conditions show specific capacities over 100 mAh/g even at 50 C rate.