As our benchmark system, we used phosphatidylcholine (PC) lipid bilayers under decreasing hydration, biologically relevant, e.g., in the desiccation and vesicle fusion contexts. Our high-resolution experimental data comprised Nuclear Magnetic Resonance order parameters for C-H bonds, S CH , which can be directly and reliably calculated from MD simulations. We presented comparisons against a dehydration dataset of all POPC lipid bilayer S CH measured in this work (see Figs. and), as well as literature dehydration datasets of all DMPC and of two POPC 49 headgroup S CH .