Using Molecular Dynamics Simulations, We Demonstrate that the Efficiency of Heat Exchange between a Solid and a Gas Can Be Maximized by Functionalizing Solid Surface with Organic Self-Assembled Monolayers (SAMs). We Observe that for Bare Metal Surfaces, the Thermal Accommodation Coefficient (TAC) Strongly Depends on the Solid-Gas Interaction Strength. for Metal Surfaces Modified with Organic SAMs, the TAC is Close to its Theoretical Maximum and is Essentially Independent from the SAM-Gas Interaction Strength. the Analysis of the Simulation Results Indicates that Softer and Lighter SAMs, Compared to the Bare Metal Surfaces, Are Responsible for the Greatly Enhanced TAC. © 2013 American Institute of Physics.