Ion-sieve adsorbents are effective materials in practical applications for extracting liquid lithium. However, it is greatly suppressed in adsorption capacity and selectivity (Li/Mg) under natural near-neutral conditions of seawater or salt lakes, due to the interference of in situ released H + and Mg 2+ impurity. This paper proposes an adsorbent with a microenvironment-modulating function as a solution. The introduction of quaternary ammonium groups into the carrier accelerates the migration of H + , while preventing the diffusion of Mg 2+ by electrostatic repulsion. Besides, it can also prestore OH − , effectively consuming the generated hydrogen ions in situ. Based on the rational design, the alkali consumption of the microenvironment-modulating strategy is dramatically reduced to 1/144 of the traditional alkali-adding method. Additionally, adsorption performance is significantly promoted under natural pH conditions, with a maximum 33 times higher separation factor (selectivity) and 4 times higher adsorption capacity than commercial ion-sieve adsorbents. This development indicates the feasibility of using microenvironment modulation for effective lithium extraction and inspires the development of next-generation highperformance adsorbents.