wide range of applications including biomimetic camouflage, [1,2] optical patterning, [3,4] optical data storage, [5,6] display devices, [7,8] electrochromic devices, [9,10] colorimetric sensors, [11,12] and so forth. At present, there are various building blocks to construct the SCNMs, such as photonic crystals, semiconductor nanoparticles, fluorescent molecules, and partial organic photoresponse molecules and their colors are alterable through Bragg diffraction, [13,14] photoluminescence, [15,16] electrochromism, [17,18] and other stimulating means. To date, much effort has been devoted to the fabrication of the SCNMs. Kim and co-workers [19] reported a facile and practical method for the fabrication of highly transparent colloidal photonic crystal films that can show multi ple colors through the overlapping of distinct layers. Rogach and co-workers [20] developed an optical approach to highly align emissive CdSe/CdS core-shell semiconductor nanorods (NRs) and the ordered area can display the color change. Zhu and co-workers [21] reported the design of multicolor fluorescent polymers that shown a color palette from blue to orange under similar excitation conditions. Although these SCNMs can exhibit a variety of colors, it still remains a big challenge to obtain richer colors in a wide spectrum, which impedes their potential applications like full-color electronic paper and electronic device screens.Noble metal nanoparticles are well known for their unique optical properties arising from the surface plasmon resonance (SPR). They usually generate abundant plasmonic colors by precisely modulating the SPR that highly depends on their sizes, morphologies, compositions, and dielectric environment. [22][23][24][25] Compared to other optical colors, the plasmonic color has distinctive optical performance including high color contrast, high resolution, and everlasting colors. [26] More importantly, full colors covering the whole range of the visible light can be obtained by selecting suitable plasmonic materials and nanostructure. For example, Chu and co-workers [2] reported reversible full-color plasmonic cell/display by electrochemically controlling the structure of an gold (Au)-Ag core-shell nanodome array. Kobayashi and co-workers [27] reported a "voltagestep method" to successfully design a multicolor electrochromic device with electrochemically size-controlled Ag nanoparticles.Due to their abundant optical colors, durable color generation, and high refreshing rate, smart chromic nanomaterials (SCNMs) have been employed in various applications. However, most SCNMs often require multicomponent materials, precise morphology control, and complicated modulation to realize multicolor changes, which limits their widely practical applications. In the present study, a simple and effective strategy is demonstrated to achieve the flexible and cost-effective multicolor gold nanorods (Au NRs)/ polymer hybrid film, by tuning macroscopic-oriented Au NRs in films and a synergy of polarization-dependent surface plasmon resonance. ...