Upon mixing with metal ions such as Cd II , Tb III , Cu II , Ni II , Pb II , Zn II , and Co II at pH 10.0, solutions of silver nanoparticles (AgNPs) coated with calix[4]arene-p-tetrasulfonate (CAS-AgNP) exhibited multi-coloration from yellow to orange, violet, and green, depending on the metal elements present, which allowed for visual discrimination of the ions. This is contrary to the AgNP sensors exhibiting a uniform color change from yellow to red upon binding of a receptor molecules at the surface of AgNPs to an analyte. The TEM images of the samples obtained from the resultant solution showed two regions. First, a region where CAS-AgNPs assembled on the surface of the metal hydroxides. The size of the hydroxide crystals varied from 50 to 200 nm with the type of metal element present, and roughly correlated with the extinction band of the aggregated AgNPs. Second, the amorphous region in which CAS-AgNPs dispersed randomly. The difference in the amount of the crystal region and the area seemed to lead to the multi-coloration.