High-voltage cathode LiMn1.5Ni0.5O4 particles with average size of approximately 2 pm were prepared using a two-step process. Low-temperature magnetic measurements indicated them as ferrimagnetic materials with high Neel temperature (146.5 K) and high magnetization (107 emu/g at 4.5 K) that closely approximates the theoretical value of the stoichiometric LiMn1.5Ni0.5O4 compound. Because of their high-purity and high crystallinity, their redox signals were observed only around 4.7 V. Their low-rate capacity was sufficiently high (about 140 mAh/g at 0.1 C). Their capacity retention after the 100th cycle was higher than 95%. In spite of the low specific surface area of the LiMn1.5Ni0.5O4 particles, they exhibited high reversible capacity even at a high current rate. Additionally, the in-situ X-ray diffraction was conducted to elucidate the reaction process, which indicated that the electrochemical reaction progresses reversibly with two consecutive two-phase reactions. The lattice parameters of three corresponding phases remained almost unchanged on the reactions (0.8165, 0.8087, and 0.8000 nm). The presence of the intermediate phase might give the relaxation of the structural variation during the electrochemical reaction.