||Self-assembly of organic block molecules can give rise to the various nanostructures such as spheres, cylinders and vesicles as well as the nanotemplates for fabrication of nanohybrids. For the organic scaffolds, incorporation of a specific block with desired functions into molecular architecture allows us to manipulate a variety of functional nanomaterials. Recently, we have developed the supramolecular nanoprobes based on the self-assembly of amphiphilic block molecules in response to the metal ions and inorganic nanoparticles which results in the drug- and imaging agent-loaded nanohybrids. Interestingly, the metal-binding process of amphiphiles induced nanoassemblies even below the CMCs, and the binding stoichiometry affected the morphologies of the resultant nanostructures. In addition, the bioconjuagated block molecules with assembly-monitoring fluorophore pendant showed the solution-state molecular organization within the nanoaggregates and specific fluorescence turn-on or turn-off response as a function of metal ion. In this talk, the fabrication of supramolecular nanoprobe for metal ion sensing in aqueous solution and its applications toward live cell imaging and antimicrobial agent will be discussed. In addition, the control of nanolocation of inorganic nanoparticles within the supramolecular hybrids will be presented.