Liquid organic hydrogen carriers (LOHCs) offer a promising solution for global hydrogen infrastructure, but their practical application faces two key challenges: sluggish dehydrogenation processes and the reliance on catalysts with high noble metal loadings. This study presents a scalable approach to reduce noble metal usage while maintaining high catalytic activity. We synthesized an ultralow Pt content (0.1 wt%) catalyst using γ‐Al2O3‐based pellet support with atomic layer deposition (ALD) of TiO2. Advanced characterization techniques reveal that the thin ALD‐TiO2 shell provides a heterogeneous interface, confining electronically rich Pt‐nanoparticle ensembles. The catalyst outperforms both equivalent Pt‐content catalysts and a commercial 0.5 wt% Pt/γ‐Al2O3 catalyst in homocyclic LOHC dehydrogenation. This study provides insights into the beneficial role of ALD‐engineered interfaces for catalytic supports and offers an efficient approach for scalable production of low‐noble‐metal‐content catalysts, with implications for various catalytic processes.