Liquid crystal elastomers (LCEs) are promising actuating materials and potential enablers of robust flexible devices. Employing directed self-assembly methods, the inherent anisotropy of nematic liquid crystals can be exploited with spatial and hierarchical patterning of the director profiles. The overarching theme of this work is the exploration and enablement of the functional utility of liquid crystalline elastomers. The research reported hereafter has focused on 1) light control enabled by concurrent shape and color change in cholesteric liquid crystal elastomers and 2) cyclic mechanical examination of the deformation of liquid crystalline elastomers to load. Detailing a facile approach to synthesizing cholesteric liquid crystalline elastomers (CLCEs) that upon heating, exhibit thermochromism. The selective reflection inherent to this phase is thermally tuned more than 200 nm in these solid films, across the visible spectrum. The optical response is directly correlated to thermomechanical expansion of the CLCE film thickness. Broadening of the bandwidth of the selective reflection of the CLCEs is achieved with the incorporation of photosensitive chiral dopants that introduce heterogeneity in the pitch distribution. The mirror-like reflection of this CLCE film is also thermochromic, shifting from the visible to infrared. When combined with the mechanical deformation of voxelated nematic LCE, the thermochromic response of the CLCE produces solid-state elements with concurrent variation of specular and diffuse reflectance. These results demonstrate distinctive potential opportunities for liquid crystal elastomers to control light enabling new application in textiles, optics, and architecture. This work additionally characterizes the stimuli response of nematic liquid crystalline elastomers (NLCEs) prepared with the same synthetic method, exhibiting unprecedented mechanical deformations of nearly 500% strain. Accordingly, this examination seeks to elucidate the mechanical response of NLCEs prepared through chain transfer reactions with diacrylate liquid crystal monomers. The mechanical response to load is explored above and below the yield point. The contribution of higher order patterns, nascent to this material chemistry, are considered and partially inform the distinctive mechanical response. This work assesses the relevance of these materials as flexible substrates for electronic devices and other implementations that could exploit the nonlinear mechanical deformation.