Supramolecular assemblies composed of nanomaterials and mediated by DNAs are a special class of superstructures that serve various functions, such as drug and gene delivery, providing a platform for bioreactions and as photodynamic and photothermal therapeutic agents depending upon the nanomaterial/s used. This work has demonstrated the formation of carbon dots (CD) and gold nanoparticle (AuNP)-based fluorescent supramolecular assemblies mediated by DNAs (helix, i-motif, and G-quadruplex). The CDs and the AuNPs have paired up as energy donors and acceptors, helping to understand the network formation spectroscopically. Partial complementary G-quadruplexes and i-motif DNAs were attached to the surface of the synthesized CDs and AuNPs, respectively, which were allowed to interact, resulting in the formation of fluorescent sheet-like structures. These sheets tear from all directions at acidic pH (=5) and show 3D compaction at pH 8.5. It is also observed that photosensitization of the CDs gets slightly enhanced upon DNA grafting and further on incorporation of the DNA-functionalized AuNPs in the network.