In order to evaluate the impact of interface curvature on the heat transfer between nanoscale-gold and water, we modeled in atomistic detail four nanoscale gold-water interfaces of different curvatures (Figure ): three spherical AuNPs with diameters (d) of 3, 5, and 10 nm, as well as a planar gold-water interface to represent the zero curvature limit. To estimate the thermal interface conductance we performed steady-state non-equilibrium molecular dynamics simulations in which the gold structure was subjected to a constant heat power, Q, while an outer region of water was maintained at 300 K as a heat sink (Figure ), approximating plasmonic heating of gold under continuous-wave laser stimulation. Under these conditions, the steady-state temperature profile in the direction normal to the interface between gold and water exhibits a temperature jump (∆T ) (Figure ), which is inversely proportional to the thermal interface conductance, G, where q = Q/A is the heat flux across the interfacial area A, which is taken as the gold surface area: A = πd 2 for spherical AuNPs with diameter d and A = 2L x L y for the planar gold surface. L x and L y are the lateral dimensions of the gold surface within the simulation cell, and the factor of two accounts for the fact that two sides of the planar surface are exposed to solvent. To consider the effects of temperature, we conducted simulations under various heating powers (Q, Table , Supporting Information). Note that in some cases, the heating caused the AuNPs to thermally expand (Table , Supporting Information), which was accounted for when computing the thermal interface conductance.