AbstractOptical metamaterials are artificially engineered architectures that exhibit desired optical properties not found in nature. Bespoke design requires the ability to define shape, size, orientation, and composition of material structures on the nanometer length scale. Bottom‐up self‐assembly methods, such as block copolymer (BCP) templating, offer unique pathways to tailored features, at spatial resolution not routinely achieved by conventional top‐down techniques. In this review, the authors provide the general readership with basic concepts of the underlying fabrication processes and examine optical phenomena arising from BCP‐derived metamaterials and nanoresonators, with both dielectric and plasmonic characteristics. A number of diverse structural conformations designed by BCP templating and their implementation in optical devices is evaluated. The discussion includes 3D metamaterials, such as gyroidal and hyperbolic arrangements, as well as 2D metasurfaces. Based on recent developments in exploring these emerging structural and material configurations, the review further highlights unexplored opportunities offered by BCP self‐assembly for novel metamaterials and metasurface devices.