Compact gas inclusion in hydrates presents not only fascinating science but also wide-ranging applications in sustainable energy and environmental technologies. The surface of hydrates dictates many essential phenomena underlying hydrate-based processes such as hydrate nucleation and growth, mass transfer, heat transfer, agglomeration, adhesion, and adsorption. Thus, surface science falls within the core of hydrate science and engineering. This paper covers an insight perspective on surface science related to the research and development of hydrate-based sustainable technologies. We present insightful molecular views of hydrate surfaces with a focus on the interfacial premelting, and discuss how new fundamental advances benefit the sustainable engineering in the areas of greener and chemical-free flow assurance, energy-efficient gas storage, carbon capture and storage, and recovery of methane (low-carbon energy) from natural hydrates. We highlight the prospects and challenges as well as stimulate future studies on this important topic.