Correlations of the shear viscosity of quartz nanofluids with particle concentration, particle size, and temperature were investigated with molecular dynamics simulations and density functional theory (DFT) calculations. A new understanding to the experimentally concluded correlations was addressed in terms of microscopic particle-water interfacial interaction in three aspects. First, the viscosity of quartz nanofluids at different particle concentrations, particle sizes, and temperatures were simulated using the equilibrium molecular dynamics simulations method to reproduce the experimental observations. At the same particle size, the nanofluid viscosity decreases significantly with temperature and increases with nanoparticle volume concentration, and at the same volume concentration, the nanofluid viscosity increases with the decrease of particle size. Second, DFT calculations confirm a stronger particle-water interaction than that among water molecules. The important role of particle-water interaction in the viscosity determination of nanofluids was revealed. Finally, a correlation was proposed to fit the simulated results and compared with earlier two-parameter correlations. One parameter in the correlation is indeed a constant, while the other is a function of SiO2-water interaction energy. Our study proposes a physical basis for the experimentally concluded correlations on the viscosity of nanofluids.© 2022. The Author(s).