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Phase change through boiling is used in a variety of heat-transfer and chemical reaction applications.[1–7] The state of the art in nucleate boiling has focused on increasing the density of bubble nucleation using porous structures and microchannels [8–12] with characteristic sizes of tens of micrometers. Traditionally, it is thought that nanoscale surfaces will not improve boiling heat transfer, since the bubble nucleation process is not expected to be enhanced by such small cavities.[13–15] In the experiments reported here, we observed unexpected enhancements in boiling performance for a nanostructured copper (Cu) surface formed by the deposition of Cu nanorods on a Cu substrate. Moreover, we observed striking differences in the dynamics of bubble nucleation and release from the Cu nanorods, including smaller bubble diameters, higher bubble release frequencies, and an approximately 30-fold increase in the density of active bubble nucleation sites. It appears that the ability of the Cu surface with nanorods to generate stable nucleation of bubbles at low superheated temperatures results from a synergistic coupling effect between the nanoscale gas cavities (or nanobubbles [16–18]) formed within the nanorod interstices and micrometer-scale defects (voids) that form on the film surface during nanorod deposition. For such a coupled system, the interconnected nanoscale gas cavities stabilize (or feed) bubble nucleation at the microscale defect sites. This is distinct from conventional-scale boiling surfaces, since for the nanostructured surface the bubble nucleation stability is provided by features with orders-of-magnitude smaller scales than …