“…In the past few years, surface-enhanced Raman scattering (SERS) has gained increasing popularity in authentication, , detections, , and diagnostics. , Apart from its high sensitivity, SERS possesses intrinsic advantages in comparison with other spectral techniques, including highly resolved spectral bands, alleviated photobleaching, as well as operation over a wide range of excitation wavelengths. These essential features suggest the capability of SERS fingerprint in barcoding and anticounterfeiting applications. − As an optical technique that depends on electromagnetic field enhancement from plasmonic nanostructures, preparation of plasmonic nanostructures becomes an indispensable step toward those emerging applications. , Although tremendous efforts have been devoted to fabrication of effective plasmonic substrates by self-assembly, − direct wield and growth of plasmonic building blocks as secondary structural domains suggests a straightforward route to plasmonic nanostructures bearing intense built-in hotspots. , However, this pathway has proved to be very difficult to achieve because nanocrystal growth principally yields symmetrical nanocrystals with simple morphologies due to thermodynamic preference. Furthermore and importantly, single hierarchical nanostructures that eradicate fluctuation of nanoparticle spacing may afford a steadier enhancement for Raman scattering. − Therefore, the development of a growth pathway to plasmonic hierarchical nanostructures are in high demand from both fundamental and technological aspects.…”