Many elements required for understanding, designing, and realizing disordered plasmonic assemblies with new or unusual combinations of properties are being developed and becoming widely accessible. Dynamic covalent bonding chemistries can be leveraged to synthetically tune reversible, chemically orthogonal colloidal interactions, paving the way for programmed assembly of disordered gel structures that can be reproducibly cycled between organized and disassembled states while avoiding uncontrolled aggregation, phase separation, and precipitation. Without the constraints of an ordered superlattice structure, gels can readily accommodate building blocks with different sizes and shapes, expanding their functional design space. Assemblies with hierarchical compositional disorder are now possible owing to synthetic methods for creating plasmonic metal oxide nanocrystals with LSPR that can be tuned from visible to mid-infrared with doping or particle composition. Though linked colloidal gels provide advantages for integrating building blocks of different shapes and sizes, 54 assembly protocols using liquid-air and subphase interfaces can also integrate compositionally distinct nanocrystals into monolayer metasurfaces or multilayer superlattices. Convergence of these experimental capabilities is timely given the recent development of freely available computational electromagnetic simulation methods capable of treating large disordered assemblies. These approaches, when paired with equilibrium or nonequilibrium simulations of assembly using coarse-grained model interactions, can yield insights into the structural origins of near-and far-field assembly properties that can inform rational design (Figure ).