The continuous increase of demand for lithium (Li) chemicals in industrial applications calls for exploring affordable Li production and sustainable options beyond land mining. Thus, aqueous resources, such as geothermal brine, salt lake brine, and seawater, play an essential role in continuous Li supply due to abundant storage and low cost. Adsorption technology is promising in Li recovery with the advantages of attaining high selectivity for Li over other major ions present in aqueous resources at low cost and low energy demand with facile synthesis processes that enable practical large-scale production. Metal-based adsorbents are conspicuous among various adsorbents for presenting the visible prospect closest to industrial applications. This review presents a comprehensive summary and critical analysis of the synthesis methods for metal-based adsorbents, the mechanisms for Li selective recovery, and the performance of Li adsorption. The advantages and challenges are discussed for different adsorbents and preparation methods. A specific focused case study on an industrial application of Al-based adsorbent production and Li recovery processes and operations on an engineering and economic scale is discussed in detail to provide a comprehensive overview of the practical industrial application of metal-based adsorbent.