Switchable optical materials, which possess reversible color and transparency change in response to external stimuli, are of wide interest for potential applications such as windows and skylights in architectural and vehicular settings or optical sensors for environmental monitoring. This thesis considers the tuning of optical properties by tailoring and actuating responsive materials. Specifically, we demonstrate the design and fabrication of tilted pillar arrays on wrinkled elastomeric polydimethylsiloxane (PDMS) as a reversibly switchable optical window. While the original PDMS film exhibits angle-dependent colorful reflection due to Bragg diffraction of light from the periodic pillar array, the tilted pillar film appears opaque due to random scattering. Upon re-stretching the film to the original pre-strain, the grating color is restored due to the straightened pillars and transmittance is recovered. Then, we develop a composite film, consisting of a thin layer of quasi-amorphous array of silica nanoparticles (NPs) embedded in bulk elastomeric PDMS, with initial high transparency and angle-independent coloring upon mechanical stretching. The color can be tuned by the silica NP size. The switch between transparency and colored states could be reversibly cycled at least 1000 times without losing the film’s structural and optical integrity. We then consider the micropatterning of nematic liquid crystal elastomers (NLCEs) as micro-actuator materials. Planar surface anchoring of liquid crystal (LC) monomers is achieved with a poly(2-hydroxyethyl methacrylate)-coated PDMS mold, leading to monodomains of vertically aligned LC monomers within the mold. After cross-linking, the resulting NLCE micropillars show a relatively large radial strain when heated above nematic to isotropic transition temperature, which can be recovered upon cooling. Finally, the understanding of liquid crystal surface anchoring under confined boundary conditions is applied to the self-assembly of gold nanorods (AuNRs) driven by LC defect structures and to dynamically tune the surface plasmon resonance (SPR) properties. By exploiting the confinement of the smectic liquid crystal, 4-octyl-4’-cyanobiphenyl (8CB), to patterned pillars treated with homeotropic surface anchoring, topological defects are formed at precise locations around each pillar and can be tuned by varying the aspect ratio of the pillars and the temperature of the system. As a result, the AuNR assemblies and SPR properties can be altered reversibly by heating and cooling between smectic, nematic and isotropic phases.