Intermetallic compound (IMC) catalysts have garnered significant attention due to their unique surface and electronic properties, which can lead to enhanced catalytic performance compared to traditional monometallic catalysts. However, developing IMC materials as high-performance catalysts has been hindered by the inherent complexity of synthesizing nanoparticles with well-defined bulk and surface compositions. Achieving precise control over the composition of supported bimetallic IMC catalysts, especially those with high surface area and stability, has proven challenging. This review provides a comprehensive overview of the recent progress in developing supported IMC catalysts. We first examine the various synthetic approaches that have been explored to prepare supported IMC nanoparticles with phase-pure bulk structures and tailored surface compositions. Key factors influencing the formation kinetics and compositional control of these materials are discussed in detail. Then the strategies for manipulating the surface composition of supported IMCs are delved. Applications of high-performance supported IMCs in important reactions such as selective hydrogenation, reforming, dehydrogenation, and deoxygenation are comprehensively reviewed, showcasing the unique advantages offered by these materials. Finally, the prevailing research challenges associated with supported IMCs are identified, including the need for a better understanding of the composition-property relationships and the development of scalable synthesis methods. The prospects for the practical implementation of these versatile catalysts in industrial processes are also highlighted, underscoring the importance of continued research in this field.