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Contemporary aspects of corrosion science are reviewed to show how insightful a surface science approach is to understand the mechanisms of corrosion initiation at the atomic and nanometric scales. The review covers experimental approaches using advanced surface analytical techniques applied to single-crystal surfaces of metal and alloys exposed to corrosive aqueous environments in well-controlled conditions and analysed in situ under electrochemical control and/or ex situ by scanning tunneling microscopy/spectroscopy, atomic force microscopy and X-ray diffraction. Complementary theoretical approaches based on atomistic modeling are also covered. The discussed aspects include the metal-water interfacial structure and the surface reconstruction induced by hydroxide adsorption and formation of 2D (hyd)oxide precursors, the structure alterations accompanying anodic dissolution processes of metals …