Thermal Conductivity of Interfacial Layers is an Essential Parameter for Determining How the Ordered Liquid Layering Around the Particle-Liquid Interface Contributes to the Unusual High Thermal Conductivity of Nanofluids. However, So Far There is No Experimental Data Regarding This Parameter. using Nonequilibrium Molecular Dynamics Simulations of an Inhomogeneous Au-Ar System in Which the Solid-Liquid Interactions Are Assumed to Be Much Stronger Than the Liquid-Liquid Interactions, We Show Explicitly that the Thermal Conductivity of a 1-Nm-Thick Interfacial Layer is 1.6∼2.5 Times Higher Than that of the Base Fluid. the Simulation Results Are Incorporated into a Three-Level Clustering Model to Calculate the Effective Thermal Conductivity of Nanofluids. the Results Show that the Contribution of the Interfacial Layer to Thermal Conductivity Enhancements Should Be Considered If There Are Particle Clusters in Nanofluids. © 2011 American Physical Society.