application of metamaterials in devices operating at optical frequencies has been hindered by high losses, high dispersion, and complex lithographic fabrication with features at subwavelength scales. The cost of such devices can be greatly reduced by exploiting the optical resonances of large-area self-assembled plasmonic nanoparticles, however their actuation has been problematic as they consist of noble metals combined with dielectrics. [8][9][10] The integration of stimuli-responsive soft materials, such as polymers and liquid crystals, can bring about significant changes in size, geometry, and refractive index. [11] Since the optical properties of the interacting plasmonic particles are highly sensitive to the interparticle separation, strong color changes can be achieved by harnessing these polymers to tune the spacing between particles. Optical switching of the plasmonic systems is especially interesting because it allows for development of more complex integrated plasmonic systems that can be optimized in real time. Plasmonic particles have high absorption cross-sections and thus efficiently convert irradiation into heat. Much research has thus explored combinations of plasmonic nanoparticles and temperature-responsive polymers. [12][13][14] In particular, there has been strong interest in using poly(N-isopropylacrylamide) (PNIPAM), a well-studied thermo-responsive polymer with a lower critical solution temperature (LCST) around 32 °C in aqueous solution. PNIPAM undergoes a phase transition to a hydrophobic state when the temperature is raised above the LCST, causing the polymer chains to contract. Upon cooling below the LCST, PNIPAM becomes hydrophilic and the chains extend into the water.This PNIPAM phase transition has been used in colloidal, 2D, and 3D structures for switchable surface enhanced Raman spectroscopy (SERS) detection, [15][16][17] drug delivery, [18] tunable color, [19][20][21] and micro-actuation. [22] However almost no work has explored light-tunable plasmonic thin-films or metasurfaces consisting of gold nanoparticles (Au NPs) using this thermoresponsive actuation. A volume phase transition of gold nanorodembedded PNIPAM hydrogel microcylinders was studied under near-infrared irradiation, [22] but showed rather slow response times ≈20 s. Other studies on Au NP-PNIPAM composite films have focused on 2D nanoparticle mats assembled at liquidliquid interfaces, [19] and superlattices formed with >50 nm thick PNIPAM shells, thicker than useful for Au NP plasmonic coupling, [21] for which light-induced actuation remains unexplored.Here we show a simple method to form large area thermoresponsive plasmonic films which achieve the fastest switching time reported for large-area composite metafilms, and exhibit Large-area dynamic switchable plasmonic metafilms composed of a network of gold nanoparticles (Au NPs) and the thermo-responsive polymer poly (N-isopropylacrylamide) (PNIPAM) are self-assembled by casting Au@ PNIPAM core-shell nanoparticles. These dense plasmonic films present an unusual opt...