Metal-organic frameworks (MOFs) containing metal nanoclusters (NCs) display great potentials, but the fabrication faces challenges because of the serious agglomeration of NCs during the MOF growth. We report a crystalline ion-triggered growth strategy for embedding AuNCs in ZIF-8. As control, when the encapsulation was triggered with other metal ions (e.g., Ca2+, Pb2+, Cd2+, Na+, Fe3+, Cu2+, and Ni2+), the AuNCs failed to be encapsulated. The quantum yields and lifetime of AuNCs were greatly enhanced after embedding in ZIF-8. The AuNCs@ZIF-8 were then successfully applied for the selective sensing of H2S both in liquid and gas phases. This crystalline ion-triggered growth strategy was easily extended to other systems, such as AgNCs@ZIF-8 and AuNCs@ZIF-67, indicating the general adaptability of this design protocol.