Strong　metal-support　interaction　(SMSI)　is　a　phenomenon　commonly　observed　on　heterogeneous　catalysts.　Here,　direct　evidence　of　SMSI　between　noble　metal　and　2D　TiB2　supports　is　reported.　The　temperature-induced　TiB2　overlayers　encapsulate　the　metal　nanoparticles,　resulting　in　core-shell　nanostructures　that　are　sintering-resistant　with　metal　loadings　as　high　as　12.0　wt%.　The　TiOx-terminated　TiB2　surfaces　are　the　active　sites　catalyzing　the　dehydrogenation　of　formic　acid　at　room　temperature.　In　contrast　to　the　trade-off　between　stability　and　activity　in　conventional　SMSI,　TiB2-based　SMSI　promotes　catalytic　activity　and　stability　simultaneously.　By　optimizing　the　thickness　and　coverage　of　the　overlayer,　the　Pt/TiB2　catalyst　displays　an　outstanding　hydrogen　productivity　of　13.8　mmol　g(cat)(-1)　h(-1)　in　10.0　m　aqueous　solution　without　any　additive　or　pH　adjustment,　with　＞99.9%　selectivity　toward　CO2　and　H-2.　Theoretical　studies　suggest　that　the　TiB2　overlayers　are　stabilized　on　different　transition　metals　through　an　interplay　between　covalent　and　electrostatic　interactions.　Furthermore,　the　computationally　determined　trends　in　metal-TiB2　interactions　are　fully　consistent　with　the　experimental　observations　regarding　the　extent　of　SMSI　on　different　transition　metals.　The　present　research　introduces　a　new　means　to　create　thermally　stable　and　catalytically　active　metal/support　interfaces　for　scalable　chemical　and　energy　applications.