In recent decades, nanodiamonds (NDs) have earned increasing interest in a wide variety of research fields, thanks to their excellent mechanical, chemical, and optical properties, together with the possibility of easily tuning their surface chemistry for the desired purpose. According to the application context, it is essential to acquire an extensive understanding of their interaction with water in terms of hydrophilicity, environmental adsorption, stability in solution, and impact on

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... l properties. In this paper, we report on a systematic study of the effects of reducing and oxidizing thermal processes on ND surface water adsorption. Both detonation and milled NDs were analyzed by combining different techniques. Temperature-dependent infrared spectroscopy was employed to study ND surface chemistry and water adsorption, while dynamic light scattering allowed the evaluation of their behavior in solution. The influence of water adsorption on their electrical properties was also investigated and correlated with structural and optical information obtained via Raman/photoluminescence spectroscopy. In general, higher oxygen-containing surfaces exhibited higher hydrophilicity, better stability in solution, and higher electrical conduction, although for the latter the surface graphitic contribution was also crucial. Our results provide in-depth information on the hydrophilicity of NDs in relation to their surface chemical and physical properties, by also evaluating the impacts on their aggregation and electrical conductance.