context: In this work, a low upper cut-off voltage of 4.5 V after an initial activation at 4.6 V is proposed and the effects of upper cut-off voltages (4.8 V and 4.5 V) on the stability of cationic/anionic redox chemistries are also studied. We demonstrate the significantly improved reversibility of cationic/anionic redox processes at the low cut-off voltage and the mitigated structural transitions from layered to rock-salt phases along with a valence decrease of Mn ions. Consequently, the LLOs present outstanding capacity/voltage stability over long-term cycling (capacity/voltage retention of 95.2%/92.2% after 200 cycles at 0.5C). The assembled mesocarbon microbead (MCMB)|LLO full cells deliver a high energy density of above 300 W h kg−1 and superior cycling/voltage stability. Compared with the previously proposed methods, this strategy is simpler and enables the use of conventional electrolytes rather than high-voltage ones that have not yet been widely commercialized up to now, which will promote the practical application of LLOs in high energy-density LIBs.