Our overall assessment is that increasing exact exchange beyond 20% has benefits on the order of ∼ 1 kcal/mol for many properties, with atomization energies as a notable exception. Further increases in the fraction of exact exchange are beneficial for problems where SIE plays a significant role but such increases have a deleterious effect on the accuracy of atomization energies. Setting the latter aside, BH&H-LYP+D3 exhibits performance that is similar to B3LYP+D3 in most cases and superior in SIE-dominated cases. Furthermore, 50% exact exchange appears to be something of an upper bound, beyond which the errors increase significantly.