Interfacial water is ubiquitous on Earth, playing a crucial role in biology, chemistry, physics, materials science, and environmental science. Multiscale, hierarchical water motions on the surface of different materials under different conditions (temperature, hydration extent, pressure, etc.) and the coupling of this motion with the substrate/solute dynamics and the influence of these couplings on the material functions are complex, long lasting, interdisciplinary research topics. We herein focus on the coupling between the picosecond dynamical onset of substrates and their surface water at temperatures lower than the freezing point (273 K) and discuss the recent progress in the study of its molecular mechanisms.