To
accurately regulate and dynamically reconstruct two-dimensional
(2D) periodic nanostructures is a great challenge but is of significance
for the development of functional integrated devices. Here, through
both chemical and physical modifications of the lithographical template
surface, a patterned dual interface of active molecular binding sites
was created, enabling flexible regulation of self-assembly of DNA-decorated
Au nanoparticles to generate 2D periodic nanostructures that feature
distinct patterns. As a proof of concept, we realized three types
of periodic structures of Au nanoparticles, including inverse structures,
ring arrays, and island arrays, through template-confined and regioselective
self-assembly processes. Besides, controllable reconstruction of the
periodic nanostructures was demonstrated through DNA-dictated assembly
of Au nanoparticles on the surface, offering a pathway to actively
manipulate their light–matter interactions. These findings
highlight the potential of heterogeneous molecular patterning of the
template surface in achieving more intricate periodic nanostructures
via surface-mediated assembly of nanoparticles over large areas.