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Abstract Dealloyed nanoporous Au membranes and spongy Au nanoparticles exhibit a set of unique structural features highly desirable for heterogeneous catalysis and electrocatalysis. In this Focus Review, we present the state‐of‐the‐art understanding of the complex mechanisms dictating the nanoscale porosity evolution during percolation dealloying of alloys and the structure‐composition‐performance correlations underpinning the catalytic behaviors of dealloyed nanoporous Au. We focus on several fundamentally intriguing but widely debated topics concerning the nature of the active sites, the dynamic surface reconstruction under reaction conditions, and the origin of catalytic selectivity toward certain reactions. We also provide perspectives on versatile dealloying‐based synthetic approaches for precise architectural tailoring of metallic nanocatalysts as well as exciting opportunities of harnessing the combined optical and catalytic properties of dealloyed nanoporous Au to drive or enhance unconventional interfacial chemical transformations.