Metrics & MoreArticle Recommendations * sı Supporting Information CONSPECTUS: In the realm of high-frequency sensing technology, the revolutionary integration and modification of novel materials such as metal−organic frameworks (MOFs), graphene, MXene, carbon nanotubes, and other advanced nanostructured materials have significantly propelled the field forward. These materials have not only broadened the scope of applications but have also markedly enhanced the capabilities of high-frequency sensors. Despite these advancements, a notable gap remains in fully understanding the relationship between the intricate structural properties of these materials and their impact on sensor performance, particularly in high-frequency contexts. Our comprehensive account seeks to bridge this gap by thoroughly analyzing the underpinning mechanisms of materials-based high-frequency sensor technology. We focus on the unique structural, electromagnetic, and surface properties of these innovative materials, emphasizing the customizable porosity and high surface area of MOFs and their influence on sensing capabilities. This Account highlights the importance of polarization theory and the strategic tailoring of materials such as MOFs, which have demonstrated potential in enhancing sensor specificity and sensitivity. Through detailed case studies and analytical explorations, we establish comprehensive guidelines for material selection in the design of high-frequency sensors. This process involves a careful consideration of target substances and specific application scenarios to ensure optimal material compatibility and performance. Additionally, we explore the significant impact of nano-and microlevel modifications in materials like MOFs on sensor characteristics, particularly in enhancing sensitivity, selectivity, and response time. The objective of our account is to elucidate the critical role that advanced materials play in the development of high-frequency sensing technology. We delve into the promising future of materials customization in highfrequency sensing, with a focus on materials that exhibit high electromagnetic properties and specialized surface characteristics. The adaptation of materials from 0D to 3D offers unique opportunities for microstructural modifications tailored to the molecular diameter of target materials, paving the way for optimal sensing system performance. This Account provides a clear and comprehensive perspective on the latest advancements and future research directions in this field. We aim to guide researchers and industry practitioners in selecting and engineering materials for superior performance in high-frequency sensing applications. By highlighting innovative research strategies and contributing to the continuous evolution of high-frequency sensing technology, our work opens new avenues for applications such as wireless transmission systems and precision biomedical monitoring. This endeavor not only pushes the boundaries of current sensing capabilities but also sets the stage for groundbreaking de...