Oxygen-deficient pristine (LMNO) and microwave-treated LiMn 1.5 Ni 0.5 O 4-δ (LMNOmic) cathode materials have been synthesized with modified thermo-polymerization synthesis technique. The XRD, XPS, CV and charge/discharge voltage profile analysis confirm that the microwave treatment enhance the electrochemical property by adjusting the lattice parameter, nickel content, and Mn 3+ content. The galvanostatic charge/discharge testing results show that LMNOmic exhibits high capacity of 133 mAh g −1 at a 0.1 C and a high retention of 95%, the LMNOmic delivered high capacity for various current rates 0.1, 0.5, 1, 2 C compared to non-microwave LMNO sample. Electrochemical impedance spectroscopy shows a gradual increase in impedance during continuous cycling, indicating a gradual formation of the cathode-electrolyte interphase (CEI) film at the active LMNO surface. The rise in impedance at the end of the 100 th cycle is about three times higher for the LMNOmic than the pristine LMNO. This work proves the urgent need for further work, specifically focusing on material design and coating and/or doping strategies that will complement microwave irradiation and ultimately permit the stabilization of the cathode-electrolyte interface upon long-term cycling. The success of such work will allow the full realization of the advantageous properties of the microwave-treatment of the LMNO and related cathode materials. LiMn 1.5 Ni 0.5 O 4-δ (LMNO) continues to attract attention and remains as one of the most promising candidates as cathode materials for rechargeable lithium-ion batteries due to its ability to provide a high operating voltage (∼4.7 V) and 3-D channels for diffusion of lithium ions in its spinel structure. [1][2][3][4][5][6][7][8][9][10][11] The advantageous properties of the LMNO such as high energy and high power density makes its suitable for heavy duty and electric vehicle applications. There is a strong demand for positive electrode materials with higher energy density Ws to realize more practical electric vehicles (EVs) and energy storage systems (ESSs). The two options to get high energy density electrode materials are either to increase the voltage (E av ) or the rechargeable capacity (Q rech ) as the energy density Ws defined as W s = ∫ Q rech d Q X E av . Moreover, the use of the high manganese (Mn) content in the cathode provides for a safer and less expensive cathode while the nickel (Ni) provides for a high voltage redox reaction of E av = 4.5 V vs Li + /Li and Q rech = 135 mAh g −1 , providing energy density of more than 600 mWh g −1 . LiMn 1.5 Ni 0.5 O 4 exists in two crystal structure forms known as ordered and disordered. The synthesis procedure of LiMn 1.5 Ni 0.5 O 4 is so crucial which determines to obtain either cation disordered face-centered cubic spinel with the space group Fd3m or its ordered variant where cation ordering on the octahedral sites lowers crystal symmetry to cubic primitive (space group P4 3 32). 6 In the disordered structure, Mn and Ni ions are more or less randomly distributed i...