Metrics & MoreArticle Recommendations CONSPECTUS: Rare earth interface structure materials (RE-ISM) play a crucial role in the field of inorganic synthesis and provide an effective means of achieving the refined utilization of rare earth elements. By capitalizing on the unique properties of rare earth, these materials are designed for functional applications at interfaces. Given the escalating energy and environmental concerns, there is an urgent need to expedite the development of efficient pathways for clean energy storage and conversion. Electrocatalytic conversion of an energetic small molecule is an efficient way of energy storage and conversion with clean energy as the carrier. However, the development of catalysts is often constrained by limitations in the catalyst system and a lack of clarity regarding synthesis and reaction processes. It provides new opportunities for the design of energetic small molecule catalytic materials by developing RE-ISM and analyzing the dynamic evolution process across time and space dimensions.In this Account, we mainly focus on the research progress in the synthesis, application, and mechanism of RE-ISM in order to effectively design high-performance materials. RE-ISM are classified into three categories based on the rare earth interface structure and the size of the substrate, following the guidance provided by the phase diagram. It mainly includes atomic interfaces, cluster interfaces, and heterstructures. By strategically designing diverse rare earth interface structures, it is feasible to effectively synthesize catalytic material systems that are tailored toward a multitude of functional applications. The synthesized RE-ISM is employed for electrocatalytic energy conversion of small molecules, offering novel prospects for catalytic electrode materials. The redox reaction process in both negative and positive grades involves the conversion of functional structural molecules through electron transfer. RE-ISM are effective catalysts for facilitating such conversion reactions. Achieving efficient construction of RE-ISM necessitates an indepth analysis of catalytic reaction mechanisms by employing in situ spectroscopy technology. The transformation process of morphology, structure, and mechanism of RE-ISM in the catalytic process was analyzed from the perspective of time resolution, spatial resolution, and spectral resolution. We elucidate the correlation between the rare earth interface interaction mechanism and the intrinsic structure based on a cognitive foundation of in situ process analysis. This provides theoretical support for the design of high-performance RE-ISM. In summary, we expect that the development of RE-ISM will provide new design ideas and insights for inorganic energy small molecule conversion materials and further promote the rapid development of high performance electrocatalytic materials.