In this topical review article, we attempt to capture recent advances in the development of sustainable hybrid nanocomposite coatings for the corrosion inhibition of structural metals. Spurred primarily by the urgent imperative of replacing hexavalent chromium but also driven by concerns regarding the environmental impact of organic solvents, materials criticality considerations, the need to maintain structural integrity and function under extreme environments, and a renewed impetus towards lightweighting, the design of new coating concepts has seen an explosion of activity. We discuss varying modes of corrosion inhibition and the drive towards multicomponent nanostructured coatings that synergistically unite multiple modes of corrosion inhibition within a single coating system. Nanocomposite coatings in which nanoparticles of one phase are dispersed within a continuous phase, usually a polymeric matrix, provide a modular design approach to multifunctional coatings provided fundamental challenges such as dispersion and compatibility can be resolved. By dint of their high surface-to-volume ratios, the incorporation of nanoparticles profoundly modifies the adjacent polymeric matrix, giving rise to an 'interphase' region with modified properties, at relatively low filler loadings. The implications of incorporating metallic, porous metal oxide, and carbon nanomaterials (graphene and carbon nanotubes) within polymeric matrices are explored with an emphasis on active corrosion inhibition. The availability of high-quality nanoparticles that are either electroactive (e.g., metals, graphene, carbon nanotubes, etc.) or are capable of serving as reservoirs for active corrosion inhibitors (e.g., porous silicon oxide, layered double hydroxides, halloysite) provides unprecedented functionality and opportunities for multifunctional coatings. The review emphasizes mechanistic considerations where these have been elucidated with a view towards developing systematic design principles for corrosion inhibition. The outlook for the future design of multimodal coatings is presented with an emphasis on the emergence of rational design of nanoparticles, advances in nanoparticle surface chemistry, high-throughput testing, materials informatics, multiscale modeling, and integrated computational materials engineering approaches.