Polyvinylpyrrolidone (PVP)-stabilized silver nanoparticles (PVP-Ag) are utilized for the detection of Hg2+ and Cr3+ ions by varying the diluting solvents, which alters the material's local surface plasmon resonance (LSPR) absorption band, forming yellow and colorless nanoparticles. Yellow PVP-Ag nanoparticles exhibit an absorption peak at 410 nm. This probe interacts with the Hg2+ ions, as a result, the intensity of the absorption peak drops, and the color changes noticeably from yellow to colorless. The colorless transparent PVP-Ag exhibits no absorption peak; however, adding Cr3+ ions causes a peak at 440 nm, thus producing a yellow color after the interaction. The TEM, DLS, and FTIR results show the interaction of materials with Hg2+ and Cr3+, which results in the change of inter-particle distance, leading to the detection of Hg2+ and Cr3+. The limits of detection (LOD) for Hg2+ and Cr3+ were determined to be 2.2 nM and 50.9 nM, respectively.