It is a new class of advanced materials combining tailorable organic ligands and inorganic building blocks that can be finely tuned with arbitrary size and shapes, [4] demonstrating unique structure-dependent properties such as gapdepended plasmonics, [1] n-doping or p-doping like properties, [5] transmutable optical and structural properties, [6] asymmetrical ion transport properties, [7] and inter/intra-plasmonic coupling. [8] While a focused ion beam (FIB) is able to program milling sites and milling depths precisely to obtain several 3D plasmene origami structures, [1,9] helical plasmonic structures have not yet been achieved.On the other hand, helical structures from plasmonic nanomaterials have recently attracted intense research due to their unique chiral optical properties. [10][11][12][13][14][15][16] For instance, a gold helix square lattice can block the circular polarization with the same handedness as the helices while transmit the other. [11] Hybrid nanoscrolls from MoS 2 or WS 2 and plasmonic Ag nanoparticles exhibited up to 500 times Plasmene is recently defined as 2D arrays of plasmonic nanoparticles, which could be fabricated by the bottom-up self-assembly approach and demonstrated a wide range of applications in sensing, energy harvesting, nanophotonics and encryption. Herein, this work further demonstrates a 3D helical plasmonic nanostructures that can be fabricated from 2D plasmene nanosheet. Inspired by chocolate curls-making process, a micro-spatulabased strategy is developed to selectively scrape substrate-supported plasmene to free space, which spontaneously folds the plasmene nanosheet into various complex helical nanostructures with controlled dimensions. 3D nanospirals can also be obtained by focus ion beam (FIB)-based lithography on free-standing plasmene. Helical plasmene structures are robust, exhibiting elastic mechanical properties and chiral optical response. This methodology represents a versatile fabrication route combining both bottom-up and topdown approaches to create soft plasmonic helical structures for potential applications in next-generation flexible nanophotonic devices.