We demonstrate that gold nanoparticles (AuNPs) are capable of unwinding double-stranded (ds) DNA. Upon unwinding, the exposed nucleobases of the separated strands adsorb onto the nanoparticle surface, resulting in the coating of the particles. The unwinding process was characterized by Atomic Force Microscopy (AFM) and absorption spectroscopy. Our results show that AuNPs initially bind to single-stranded overhangs at the duplex termini, forming dsDNA–nanoparticle dumbbells. This binding event subsequently initiates the separation of the DNA strands. As the unwinding proceeds, the nanoparticles become progressively wrapped by the unwound DNA strands, which leads to a gradual reduction in the interparticle distance within the dumbbells. This process is driven by the strong affinity of nucleobases for the gold surface. The efficiency of DNA unwinding was found to depend strongly on both nanoparticle size and temperature. These findings provide new insights into DNA-nanoparticle interactions and may facilitate the rational design of DNA–AuNP hybrid nanostructures such as dumbbell-shaped conjugates for applications in DNA-based nanoelectronics, biosensing, and self-assembled nanomaterials.