In order to elucidate the basis set dependence of the DFT based results, we computed the energy balance of the anisole-methanol dimer for di↵erent basis sets as shown in Tab. S 2. Thereby, the geometry optimization, single point energy calculation and zero-point vibrational energy correction are computed all at the same level of theory. Our harmonically corrected results are in agreement with the values provided by Heger et al. With increasing basis set size, the OH-⇡ bound dimer relative energy is estimated at about 1 kJ mol 1 . The experimental observations would be more in line with an energy di↵erence of 2 kJ mol 1 or more. Our multicomponent approach placed the relative energy at about 3.5 kJ mol 1 .