Studies of stable catalysts for non-oxidative dehydrogenation of ethane (NDE) have been challenged by coke deposition from side reactions and thermal sintering of active species. Herein, we report a catalyst mechanism that overcomes both challenges to enable highly stable, active, and selective NDE. The catalyst is made of subnanometric platinum (Pt) species (i.e., single atoms and clusters) habituated on a two-dimensional (2D) multilamellar titanium silicalite-1 (M-TS-1) zeolite nanosheet support (i.e., Pt/M-TS-1). The ultrathin (∼3 nm) M-TS-1 nanosheets provide high external surface areas, high terminal silanol/titanol (−OH) groups, and weak Lewis acid sites. The first two characteristics enhance molecular transport and Pt dispersion in the catalyst support. The third characteristic prohibits side reactions to avoid coking and create strong Pt–support interaction, leading to well-dispersed Pt species against thermal sintering. The M-TS-1 nanosheet-supported Pt catalyst exhibited durable catalytic activity and high ethylene selectivity in the NDE.