Here, we demonstrate how simulations of binary PCCHOL mixtures can be evaluated against experimental NMR spectroscopy and X-ray scattering data by interpolating through multiple CHOL concentrations. As the eect of CHOL on lipid headgroup (and its independence from acyl chain ordering) has been discussed previously, we focus here on the acyl chains; these are expected to play a larger role than the headgroup in CHOL-induced lateral membrane heterogeneity. We also evaluate the dependence of lateral diusion coecients on CHOL against pulsed eld gradient (PFG) NMR experiments 50,51 using the recent theoretical framework that allows a quantitative comparison with experiment by eliminating nite-size eects in MD simulations. With the structural and dynamic comparisons established, we then estimate the quality of four popular force elds at dierent CHOL concentrations.