In response to the climate goal of achieving carbon neutrality by 2050, efficient electrochemical energy conversion devices are garnering increasing attention. However, the enhancement of electrochemical performance using noble metal electrocatalysts, along with cost reduction and electrode fabrication, remain significant challenges. Noble metal hybrid nanostructures, possessing multiple surface functionalities, lead to outstanding electrocatalytic performances and low‐cost potential. Strain effects can bolster the bonding strength between the noble metal layers and the substrate or core layers, while simultaneously affecting electrocatalytic performance through tuning the binding strength between catalytically active sites and reactants, including intermediates. This review encapsulates the research efforts directed towards improving the performance of noble metal electrocatalysts and provides an overview of the latest advancements in controlling the surface state of noble metals by incorporating a secondary component. We discuss systematic approaches to adjusting surface strain effects on noble metals, characterization techniques, and application case studies, while extracting key design indicators for readers to consider from a macroscopic perspective. Further, we outline the challenges encountered and current solutions when advancing noble metal catalysts from theoretical mechanisms to practical use. Finally, the perspectives on the future research of noble metal surface layer control techniques were also provided.