Validation on the basis of literature data and solving the interpolation issue were central to verifying the reliability of our Langevin NEMD method. However, other technical and model-related factors that can possibly influence the Soret coefficient were also sounded out. Specifically, it was reassured that the Langevin damping constant, the width of the temperature control regions, the system size, and the cutoff radius have no systematic impact on S T (Supporting Information S2.4), which leads us to the conclusion that the Langevin NEMD method proposed here yields reliable and robust results.