While it has been previously accepted that graphene growth on metal films by chemical vapor deposition (CVD) protects the surfaces by stiffening and hardening, in this study, an unusual opposite effect is reported. Herein, we use nanoindentation to study the mechaniported. Herein, we use nanoindentation to study the mechanical behavior of graphene‐covered platinum foils. Two graphene growth recipes using undiluted and diluted methane flow are studied, aiming to achieve a bulk or a surface‐mediated graphene growth mechanism, respectively. Contrary to previous reports, a 17% decrease is observed in the elastic modulus of the Pt surfaces when covered by graphene compared to graphene‐free regions for both recipes, when using the real indentation contact area extracted via atomic force microscopy (AFM) for the estimation. By performing cross‐sectional transmission electron microscopy (TEM), subsurface multilayers responsible for the decrease in stiffness are revealed and these observations and the mechanism of layer formation are explained. Hence, in this study, it is highlighted that surface stiffening of metals by graphene CVD has exceptions, especially in the case of metals with high carbon solubility. Moreover, in this study, approaches for combining cross‐sectional TEM, topological scans from AFM, and raw load–displacement data from nanoindentation to provide a complete, multiscale elucidation of the mechanical behavior of a material surface are described.
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