Efficient and durable catalysts are essential for the practical implementation of dehydrogenation processes in liquid organic hydrogen carrier (LOHC) systems. In this study, we demonstrate that the catalytic performance of platinum (Pt)/TiO2 catalysts can be fundamentally modified via morphology-driven facet engineering of the TiO2 support for dehydrogenation of methylcyclohexane (MCH). Anatase TiO2 supports with distinct exposed facets were synthesized for a direct comparison between {001}-exposed nanosheets and {101}-dominant nanorhombic and polyhedral structures. Among these, the Pt catalyst supported on TiO2 nanosheets exhibits significantly enhanced catalytic activity and stability during MCH dehydrogenation. Comprehensive spectroscopic and adsorption analyses reveal that the two-dimensional nanosheet architecture induces strong interfacial electronic interactions, stabilizes metallic Pt species, and promotes favorable surface acidity. This architecture also improves reactant adsorption and accessibility of active sites. Consequently, the Pt/nanosheet-TiO2 catalyst delivers superior intrinsic activity and excellent morphological stability under reaction conditions. This study highlights support morphology and facet exposure as key design parameters to control interfacial chemistry and catalytic functionality, providing a general strategy to advance the development of LOHC-based hydrogen storage technologies. © 2026 The Author(s). Small Science published by Wiley-VCH GmbH.