Using the newly developed organic-inorganic colorant membrane is an attractive approach for the optical detection, selective screening and removal, and waste management recovery of highly toxic elements, such as Hg(II) ions, from water sources. In the systematic mesosponge optical sinks (MOSs), anchoring organic colorants into 3D, well-defined cage cavities and interconnected tubular pores (10 nm) in the long microscale channels of membrane scaffolds enhances the requirements and intrinsic properties of the hierarchal membrane. This scalable design is the first to allow control of the multifunctional processes of a membrane in a one-step screening procedure, such as the detection/recognition, removal, and filtration of ultratrace Hg(II) ions, even from actual water sources (i.e., tap, underground). The selective recovery, detection, and extraction processes of Hg(II) ions in a heterogeneous mixture with inorganic cations and anions as well as organic molecules and surfactants are mainly dependent on the structure of the colorant agent, the pH conditions, competitive ion-system compositions and concentrations, and Hg-to-colorant binding events. Our result shows that the solid MOS membrane arrays can be repeatedly recycled and retain their hierarchal mesosponge sink character, avoiding fouling via the precipitation of metal salts as a result of the reuse cycle. The Hg(II) ion rejection and the permeation of nonselective elements based on the membrane filtration protocol may be key considerations in water purification and separation requirements. The selective recovery process of Hg(II) ions in actual contaminated samples collected from tap and underground water sources in Saudi Arabia indicates the practical feasibility of our designed MOS membrane arrays.