geometric parameters were fabricated to provide varied reflection spectra and surface enhanced Raman scattering (SERS) signals. [11] These types of plasmonic substrates can be applied as integrated platforms in optical biosensing, [12] telecommunication, [13] surface-enhanced spectroscopy, [14] and light harvesting. [15] Material gradients are also a valuable material research tool that allows highthroughput and cost-effective screening material properties in a minimum amount of time. To speed up materials discovery, an artificial library containing gradients of the material parameters of interest (morphology, composition, surface property, etc.) under similar condition is experimentally created, [16] and rapid, local, and automated measurements are performed to establish a material parameter-property relationship. [1,17] Such a methodology is generally faster and less expensive than traditional (e.g., "one material at a time") approach. Since all characterizations are carried out on the same library samples with the same measurement tools over a short time period, most systematic errors are eliminated, thus generating a comprehensive and reliable data set. In particular, plasmonic library based on ordered and well-defined noble metal gradient nanostructures has been extensively studied. Plasmonics, known as coherent oscillations of conduction electrons on a metal surface excited by electromagnetic radiation at a metal-dielectric interface, constitute one of the most important building blocks of contemporary nanoscience and nanotechnology. [18] Plasmonic properties are strongly dependent on the size, shape, orientation, and interspacing of the nanostructures. [19] The study of geometric-dependent (or compositional) optical properties and the optimization of nanofabrication protocols can be greatly facilitated by establishing plasmonic libraries.The development of plasmonic library is basically determined by the nanofabrication techniques. Conventional lithography (hard lithography) techniques, such as electron beam lithography (EBL) and focused ion beam lithography (FIB), are most widely used to introduce ordered and well-defined gradient nanostructures. While these techniques are capable of precise control over the size, shape, and spacing of metallic nanostructures, they are limited by high cost, low throughput, and requirement of sophisticated equipment. [9,10,17,20] Recent research has been focused on developing low-cost and efficient unconventional techniques to produce gradient plasmonic structures (GPSs). Fery and co-workers used a dip-coating Gradient plasmonic nanostructures are produced by a straightforward and powerful fabrication strategy-deposition on curved nanomask (DCNM), a physical vapor deposition on a curved mask substrate covered with a mono layer of closepacked nanospheres. The feasibility of the DCNM strategy is demonstrated by producing wellordered Ag gradient single/double nanotri angle (NT) arrays with continuously adjustable color, extinction, localized sur face plasmon resonance wavelen...