Carbon dots are an emerging class of nanomaterials that has recently attracted considerable attention for applications that span from biomedicine to energy. These photoluminescent carbon nanoparticles are defined by characteristic sizes of <10 nm, a carbon‐based core and various functional groups at their surface. Although the surface groups are widely used to establish non‐covalent bonds (through electrostatic interactions, coordinative bonds, and hydrogen bonds) with various other (bio)molecules and polymers, the carbonaceous core could also establish non‐covalent bonds (ππ stacking or hydrophobic interactions) with π‐extended or apolar compounds. The surface functional groups, in addition, can be modified by various post‐synthetic chemical procedures to fine‐tune the supramolecular interactions. Our contribution categorizes and analyzes the interactions that are commonly used to engineer carbon dots‐based materials and discusses how they have allowed preparation of functional assemblies and architectures used for sensing, (bio)imaging, therapeutic applications, catalysis, and devices. Using non‐covalent interactions as a bottom‐up approach to prepare carbon dots‐based assemblies and composites can exploit the unique features of supramolecular chemistry, which include adaptability, tunability, and stimuli‐responsiveness due to the dynamic nature of the non‐covalent interactions. It is expected that focusing on the various supramolecular possibilities will influence the future development of this class of nanomaterials.