The study of the formation, characterization, and functionality of isolated surface hydrides on solid materials is a formidable task because of the complexity of solid surfaces and the difficulty of analyzing structures in solids. Herein, we found the formation of indium (In) hydride species supported by CHA zeolites. The In hydrides were formed by treatment of an In-exchanged CHA zeolite (In-CHA) with H-2 at high temperatures (>773 K). In situ Fourier transform infrared (FTIR) spectroscopy and density functional theory (DFT) calculations revealed that an [InH2](+) ion on a framework anionic site is a plausible structure. In-CHA exhibited high selectivity and durable catalytic activity for the nonoxidative dehydrogenation of ethane for at least 90 h. Kinetic and in situ spectroscopic studies as well as transition state (TS) calculations suggested that [InH2](+) ions serve as catalytically active sites for selective dehydrogenation using In-CHA.