<p>Metamaterials are artificially structured materials which attain their unconventional macroscopic properties from their cellular configuration rather than their constituent chemical composition. The judicious design of this cellular structure opens the possibility to program and control the optical, mechanical, acoustic, or thermal responses of metamaterials. This Ph.D. dissertation focuses on scalable design and manufacturing strategies for optical and mechanical metamaterials.<br> <br> </p> <p>The fabrication of optical metamaterials still relies heavily on low-throughput process such as electron beam lithography, which is a serial technique. Thus, there is a growing need for the development of high-throughput, parallel processes to make the fabrication of optical metamaterials more accessible and cost-effective. The first part of this dissertation presents a scalable manufacturing method, termed “roll-to-roll laser induced superplasticity” (R2RLIS), for the production of flexible optical metamaterials, specifically metallic near-perfect absorbers. R2RLIS enables the rapid and inexpensive fabrication of ultra-smooth metallic nanostructures over large areas using conventional CO₂ engravers or inexpensive diode lasers. Using low-cost metal/epoxy nanomolds, the minimum feature size obtained by R2RLIS was <40 nm, facilitating the rapid fabrication of flexible near-perfect absorbers at visible frequencies with the capability to wrap around non-planar surfaces.</p> <p> </p> <p>The existing approaches for designing mechanical metamaterials are mostly <i>ad hoc</i>, and rely heavily on intuition and trial-and-error. A rational and systematic approach to create functional and programmable mechanical metamaterials is therefore desirable to unlock the vast design space of mechanical properties. The second part of this dissertation introduces a systematic, algorithmic design strategy based on Voronoi tessellation to create architected soft machines (ASMs) and twisting mechanical metamaterials (TMMs) with programmable motion and properties. ASMs are a new class of soft machines that benefit from their 3D-architected structure to expand the range of mechanical properties and behaviors achievable by 3D printed soft robots. On tendon-based actuation, ASMs deform according to the topologically encoded buckling of their structure to produce a wide range of motions such as contraction, twisting, bending, and cyclic motion. TMMs are a new class of chiral mechanical metamaterials which exhibit compression-twist coupling, a property absent in isotropic materials. This property manifests macroscopically and is independent of the flexible material chosen to fabricate the TMM. The nature of this compression-twist coupling can be programmed by simply tuning two design parameters, giving access to distinct twisting regimes and tunable onset of auxetic (negative Poisson’s ratio) behavior. Taking a metamaterial approach toward the design of soft machines substantially increases their number of degrees of freedom in deformation, thus blurring the boundary between materials and machines.</p>