Metamaterials are artificial materials designed to create optical properties that do not exist in nature. They are assemblies of subwavelength structures that are tailored in size, shape, composition, and orientation to realize the desired property. Metamaterials are promising for applications in diverse areas: optical filters, lenses, holography, sensors, photodetectors, photovoltaics, photocatalysts, medical devices, and many more, because of their excellent abilities in bending, absorbing, enhancing and blocking light. However, the practical use of metamaterials is challenged by the lack of plasmonic materials with proper permittivity for different applications and the slow and expensive fabrication methods available to pattern sub-wavelength structures. We have also only touched the surface in exploring the innovative uses of metamaterials to solve world problems. In this thesis, we study the fundamental optical properties of metamaterial building blocks by designing material permittivity. We continuously tune the interparticle distance in colloidal Au nanocrystal (NC) solids via the partial ligand exchange process. Then we combine top-down nanoimprint lithography with bottom-up assembly of colloidal NCs to develop a large-area, low-cost fabrication method for subwavelength nanostructures. Via this method, we fabricate and characterize nano-antenna arrays of different sizes and demonstrate metasurface quarter wave-plates of different bandwidth, and compare their performances with simulation results. We also integrate the metasurfaces with chemically- and mechanically-responsive polymers for strong-signal sensing. In the first design, we combine ultrathin plasmonic nanorods with hydrogel to fabricate optical moisture sensors for agricultural use. In the second application, we design mechanically tunable Au grating resonances on a polydimethylsiloxane (PDMS) substrate. The dimensions of Au grating are carefully engineered to achieve a hybridized, ultrasharp, and ultrasensitive resonance peak.