Concentration of ions and molecular species from water on solid surfaces is a topic covering a wide range of scientific and practical applications for such purposes as the removal of toxic compounds and the collection of noble elements and molecules. The adsorption-based process is one of the most promising strategies; therefore, searching for and designing adsorbents for target ions and molecules have been actively conducted. Layered inorganic solids and their derivatives are promising adsorbents with the following advantages: a) large surface area derived from well-defined nanostructures composed of an ultrathin layer (a so-called "nanosheet"), b) chemical and thermal stabilities when compared with their organic counterparts, and c) material diversity. [1] As for the ion-exchange selectivity on layered inorganic solids, it has been recognized that anions with higher charge and smaller size are preferred on layered double hydroxides.[2]Concentration of cationic species, especially heavy metals and radioactive ions, on ion-exchangeable layered materials, such as smectite clays, [3] synthetic micas, [4] layered metal phosphates, [5] and layered titanates, [6] has been studied so far. A wide variety of materials are available; [1,7] therefore, it is worth investigating the concentration of various cations on layered inorganic solids. To concentrate heavy-metal ions, the organic modification of layered [8] and mesoporous materials [9] has been conducted, and it was found that thiol groups attached on the solid surface played a role in the adsorption of Hg 2+ . Because of the demands for the environmental purification and collection of noble-metal ions, there is a need for selective ion-exchange processes for a wide variety of target elements using environmentally friendly materials.[10]Herein, we report the selective and effective adsorption of Zn 2+ on a layered silicate, magadiite. [11] Zinc is an element essential for life; it exists in seawater (at the concentration of 0.4 ppb) [12] and has been shown to be harmful to human and aquatic animal health. [13,14] Magadiite is a naturally occurring layered alkali silicate [11d] that can be readily synthesized by a simple hydrothermal reaction between silica, sodium hydroxide, and water. [11a,b] Therefore, the successful procedure reported herein opens up a new opportunity for collecting Zn 2+ from seawater. In addition, we found that the concentration of Zn 2+ can be achieved even in the presence of Cd 2+ , which often competes and disturbs the concentration and detection of Zn 2+ . [15,16] The characteristics of magadiite and other adsorbents examined in this study (another kind of Na + -type layered alkali silicate, octosilicate, [17] a naturally occurring Na +