During the past few decades, the construction of discrete metallomacrocycles via coordination-driven self-assembly has attracted considerable attention since this strategy has proven to be a simple yet highly efficient approach for the preparation of metallomacrocycles with predetermined shapes and sizes. In addition to comprehensive research on the design and synthesis of metallomacrocycles, investigation of the applications of self-assembled metallomacrocycles is developing rapidly. More recently, increasing attention has been drawn to exploiting new applications of metallomacrocycles, thereby promoting the development of supramolecular chemistry and materials science. This chapter focuses on recent progress on the applications of self-assembled metallomacrocycles in the fields of catalysis and sensing. The synthesis and characterization of these self-assembled metallomacrocycles are also discussed.