DNA nanostructures as scaffolds for drug delivery, biosensing, and bioimaging are hindered by its vulnerability in physiological settings, less favorable of incorporating arbitrary guest molecules and other desirable functionalities. Noncanonical self-assembly of
DNA nanostructures with small molecules in an alternative system is an attractive strategy to expand their applications in multidisciplinary fields and is rarely explored. This work reports a
nitrogen-enriched
carbon dots (NCDs)-mediated
DNA nanostructure self-assembly strategy. Given the excellent photoluminescence and photodynamic properties of NCDs, the obtained
DNA/NCDs nanocomplex holds great potential for bioimaging and anticancer
therapy. NCDs can mediate
DNA nanoprism (NPNCD ) self-assembly isothermally at a large temperature and pH range in a
magnesium-free manner. To explore the suitability of NPNCD in potential biomedical applications, the cytotoxicity and cellular uptake efficiency of NPNCD are evaluated. NPNCD with KRAS
siRNA (NPNCD K) is further conjugated for KRAS-mutated
nonsmall cell lung cancer therapy. The NPNCD K shows excellent gene knockdown efficiency and anticancer effect in vitro. The current study suggests that conjugating NCDs with programmable
DNA nanostructures is a powerful strategy to endow
DNA nanostructures with new functionalities, and NPNCD may be a potential
theranostic platform with further fine-tuned properties of CDs such as near-red fluorescence or photothermal activities.