Pure-phase and well-crystallized spinel LiAl0.05Mn1.95O4 powders were successfully synthesized by a simple ultrasonic assisted rheological phase (UARP) method. The structure and morphology properties of this as-prepared powder compared with the pristine LiMn2O4 and LiAl0.05Mn1.95O4 obtained from the solid-state reaction (SSR) method were investigated by powder X-ray diffraction (XRD) and scanning electron microscopy (SEM). The electrochemical properties focused on the LiAl0.05Mn1.95O4 by this new method have also been investigated in detail. According to these tests results, it is obviously to see that the newly prepared sample delivers a relatively high initial discharge capacity of 111.6mAhg−1, presents excellent rate capability and reversibility, and shows good cycling stability with capacity retention of 90.6% after 70 cycles. Meanwhile, the electrochemical impedance spectroscopy (EIS) investigations were employed to study the electrochemical process of Li+ ions with the synthesized LiAl0.05Mn1.95O4 electrode in detail.