In this Article, we present a facile microwave-assisted synthesis route for the preparation of water-soluble and high-quality CuInS2/ZnS nanocrystals (NCs) with glutathione as the stabilizer. The as-prepared CuInS2/ZnS NCs exhibited small particle sizes (~3.3 nm), long photoluminescence lifetimes, and color-tunable properties ranging from the visible to the near-infrared by varying the initial ratio of Cu/In in the precursors. The low-toxicity, highly luminescent and biocompatible CuInS2/ZnS NCs were applied to cell imaging, showing that they could be used as promising fluorescent probes. Furthermore, the CuInS2/ZnS NCs were used as the signal labels for a fluoroimmunoassay of the biomarker IL-6, showing their great potential for use as reliable point-of-care diagnostics for biomarkers of cancer and other diseases.