The tunable photoluminescent and photocatalytic properties of carbon dots (CDs) via chemical surface modification have drawn increased attention to this emerging class of carbon nanomaterials. Herein, we summarize the advances in CD synthesis and modification, with a focus on surface functionalization, element doping, passivation, and nanocomposite formation with metal oxides, transition metal chalcogenides, or graphitic carbon nitrides. The effects of CD size and functionalization on photocatalytic properties are discussed, along with the photocatalytic applications of CDs in energy conversion, water splitting, hydrogen evolution, water treatment, and chemical degradation. In particular, the enzyme-mimetic and photodynamic applications of CDs for bio-related uses are thoroughly reviewed.