Carbon dots (CDs) are a novel class of nanoparticles with excellent properties. The development of CDs involves versatile synthesis, characterization, and various applications. However, the importance of surface chemistry of CDs, especially in applications, is often underestimated. In fact, the study of the surface chemistry of CDs is of great significance in the explanation of the unique properties of CDs as well as the pursuit of potential applications. In this feature article, we do not only introduce the development of CDs in our group but also highlight their applications where surface chemistry plays a critical role.