Controlled three-dimensional chiral arrangement of plasmonic nanocomponents is crucial for understanding emergent light-matter interactions but remains challenging, particularly for heterogeneous plasmonic nanoparticles with distinct shape anisotropy. Here, using an elaborately designed DNA assembly strategy, we constructed hybrid chiral plasmonic systems integrating gold nanodisks and nanorods. Chiroptical activity arises from the asymmetric lateral displacement between them, and the sign and intensity of the circular dichroism are determined by the number and handedness of the nanorod arrangements. We reveal that this chiroptical activity originates from selective plasmonic coupling between the in-plane resonance of the nanodisks and the longitudinal resonance of the nanorods, representing an experimental realization of an extended plasmonic Born−Kuhn model. This work opens new avenues in plasmonics and nanophotonics by providing a design paradigm for constructing complex chiral architectures.

Planar assemblies of plasmonic nanoparticles have provided opportunities in various fields. This study exploits the self-assembly of gold nanorods (AuNRs) into planar, layered chiral superstructures (dodecamer) using DNA origami technology. Due to the collective plasmonic coupling modes, the dodecamers exhibit g-factors of up to +0.06, which is 4–5 times higher than those of the dextrodimers. The chiroptical property of the superstructures proved to be strongly size-dependent, exhibiting enhanced g-factors with increasing the size of AuNRs. Moreover, by excluding the averaging and close-to-racemic effects in the ensemble colloids, circular differential scattering (CDS) and circularly polarized luminescence (CPL) were studied at the single-particle level, revealing the essential role of the structural chirality of superstructure in correlating single-particle scattering with nearby dye emission. The observed correlated CDS and CPL show g-factors up to −0.17 and −0.6, respectively. These results highlight the potential of DNA origami-directed plasmonic assemblies for nanoscale chirality engineering, with applications in biosensing, chiral photonics, and metamaterials.