Gold nanoclusters (AuNCs) have been widely investigated because of their unique photoluminescence properties. However, the applications of AuNCs are limited by their poor stability and relatively low fluorescence. In the present work, we developed nanocomposites (L-Cys-AuNCs@ZIF-8) with high fluorescence and stability, which were constructed by encapsulating the water-dispersible L-Cys-AuNCs into a ZIF-8 via Zn2+-triggered growth strategy without high temperature and pressure. The maximum emission wavelength of the L-Cys-AuNCs@ZIF-8 composite was at 868 nm, and the fluorescence intensity of L-Cys-AuNCs@ZIF-8 was nearly nine-fold compared with L-Cys-AuNCs without the ZIF-8 package. The mechanism investigation by fluorescence spectroscopy and X-ray photoelectron spectroscopy showed that L-Cys-AuNCs@ZIF-8 impeded ligand rotation, induced energy dissipation, and diminished the self-quenching effect, attributing to the spatial distribution of L-Cys-AuNCs. Based on the high fluorescence efficiency of L-Cys-AuNCs@ZIF-8, a “signal off” detective platform was proposed with copper ions as a model analyte, achieving a sensitive detection limit of Cu2+ at 16.7 nM. The quenching mechanism was confirmed, showing that the structure of the L-Cys-AuNCs@ZIF-8 nanocomposites was collapsed by the addition of Cu2+. Attributing to the strong adsorption ability between copper ions and pyridyl nitrogen, the as-prepared L-Cys-AuNCs@ZIF-8 was shown to accumulate Cu2+, and the Zn2+ in ZIF-8 was replaced by Cu2+.