Spinel lithium manganese oxide LiMn2O4 and its substituted forms LiM1/6Mn11/6O4 (M=Co, Al and Ni) were prepared by ultrasonic spray pyrolysis method. As-prepared particles showed a spherical morphology and a densely congested interior structure. The geometric mean diameter was between 0.76 and 0.93μm, and the geometric standard deviation was approximately 1.33. The crystallite size was approximately 30nm, and the specific surface area of the particles ranges from 5.7 to 12.7m2/g. As-prepared particles were used as cathode active materials for lithium secondary battery and their charge/discharge properties have been investigated. As a result, it could be seen that ultrasonic spray pyrolysis is an effective method to prepare lithium manganese oxide (LiMn2O4) and its substituted forms within very short production time, which is only 4.8min in the present work.