With large specific surface area, abundant adsorption sites, flexible pore structure, and good water stability, Materials of Institute Lavoisier frameworks (MILs) have attracted increasing attention as effective environmental adsorbents. This review systematically analyzes and recapitulates recent progress in the synthesis and application of MIL-based adsorbents for the removal of aqueous heavy metal ions. Commonly used solvothermal, microwave, electrochemical, ultrasonic, and mechanochemical syntheses of MILs are first summarized and compared. Instead of focusing on adsorption process parameters, adsorption performances and governing mechanisms of virgin MILs, functional MILs, MIL-based composites, and carbonized MILs to representative metal(loid) ions (chromium, arsenic, lead, cadmium, and mercury) in water under various conditions are then systematically reviewed and discussed. In the end, this work also outlines prospects and future directions to promote the applications of MILs in treating heavy metal contaminated water.