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Lithium/aluminum layered double hydroxides (Li/Al-LDHs) have been industrially proven to be recyclable lithium adsorbents that do not dissolve upon elution, although they are hypersensitive to lithium deintercalation. In this study, the Li+ adsorption performances and structural stabilities of Li/Al-LDHs samples with different lithium deintercalation intensities are comprehensively investigated and compared to expose the influence of excessive lithium deintercalation. The characterization results demonstrate that Li/Al-LDHs are inclined