The effect of Pt on the structural evolution of nanoporous gold (NPG) is complex and is controlled by processes including secondary dealloying of Ag, surface diffusion of Au, and Pt segregation. High-resolution studies are carried out to investigate the interplay of the inherent processes. Observations such as Pt segregation at nanoligament surfaces, core-shell structures of nanoligaments, and Ag retention inside individual nanoligaments are seen at unprecedented detail using high resolution characterization techniques, including Atom Probe Tomography (APT) and Electron Energy Loss Spectroscopy (EELS). Quantitative estimates of the surface area-to-volume ratios of nanoporous layers with different Pt content indicate their relative functionalities for surface area driven applications. (C) 2018 Elsevier Ltd. All rights reserved.