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LiMn 2 O 4 (LMO) cathodes suffer from limited cycle life, resulting from Mn dissolution and side reactions between electrode and electrolyte. In this study, Sr-modified LMO is prepared by using a simple strategy. The nature and position of large-radius Sr ions are investigated, alongside their influence on the structural stability of the bulk. SrMnO 3 (SMO) is found to be enriched at grain boundaries of LMO, with MnÀ OÀ Sr bonds forming at the SMO/LMO interface. Furthermore, stable SMO alleviates the migration of Mn ions in LMO associated with structural integrity and suppresses side reactions between the electrode and electrolyte. The modified LMO cathodes maintain their structural integrity and display improved rate performance and cycling stability under harsh conditions. Remarkably, the discharge capacity of a Sr-modified LMO j j Li half-cell maintains 94.8 % at 25 °C and 79.6 % at 55 °C after 500 cycles. Consequently, enrichment of strontium at grain boundaries presents a promising strategy for developing cathodes for long-term use.