Featured by prominent flexibility and fidelity in producing sophisticated stereoscopic structures transdimensionally, three-dimensional (3D) laser printing technique has vastly extended the toolkit for delivering diverse functional devices. Yet chiral nanoemitters heavily resorting to artificial structures that manifest efficient emission and tightly confined light-mater interactions simultaneously remains alluring but dauntingly challenging for this technique at this moment. In this work, we assert the chiral photoluminescence is implemented from silver nanostructures of optical duality in one go via a twofold three-dimensional laser printing scheme. Such laser printing protocol allows the highly desired duality by simultaneously producing uniformly distributed fluorescent silver nanoclusters and aggregated plasmonic silver nanoparticles to tightly confine chiral interactions at the nanoscale. A helical emitter of 550 nm-helix-diameter as fabricated has seen a record-high luminescence anisotropic factor with the absolute value up to 0.58, which is two orders of magnitude greater than fluorescent chiral silver clusters. This method holds great promise for future versatile applications in chiroptical nanodevices.
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