Oscillating heat pipes (OHPs) provide a promising heat transfer device for a variety of applications, including the cooling of electronic devices. Recently, it has been shown that a hydrophilic, nanostructured cupric oxide (CuO) coating can significantly enhance the thermal performance of copper OHPs that use water as the working fluid. Motivated by these results, we report neutron scattering and electron microscopy (EM) measurements to investigate the interaction of water with copper-oxide surfaces on the nanoscale. Our measurements confirm earlier observations of a thin cuprous oxide (Cu2O) layer growing on a bare copper substrate followed by “grass-like” CuO nanostructures. New evidence of the nanostructure hydrophilicity is provided by EM measurements of wetting and by our high-energy-resolution elastic neutron scattering measurements, showing a continuous freezing and melting of the water in our samples over a temperature range of ∼80 K. In addition, our neutron diffraction measurements are consistent with water closest to the CuO nanostructures freezing into an amorphous solid at low levels of hydration and hexagonal ice at higher hydration. In short, our findings support a strong interaction of water with the CuO nanostructures, which could significantly affect the operation of an OHP.