The proton nuclear magnetic resonance (NMR) technique is becoming increasingly popular in various assessments of physical properties in hydrate-bearing sediments, and NMR transverse relaxation time T 2 spectra are normally converted into pore size distributions by using the NMR transverse surface relaxivity ρ 2 . However, how the NMR ρ 2 value evolves during hydrate dissociation or formation remains elusive largely due to the lack of experimental data. Thus, combined measurements of lowfield NMR and X-ray computed tomography (CT) are performed to quantify the value of NMR ρ 2 in quartzitic sands with different xenon hydrate saturations. Effects of hydrate saturation and pore habits on the value of NMR ρ 2 are analyzed, and theoretical models are correspondingly proposed. These experimental data and theoretical models are extended to NMR-based predictions of hydraulic permeabilities and water retention curves, and suggestions for the predictions are given. Results show that the value of NMR ρ 2 increases first and then decreases due to the presence of xenon hydrate in pores of quartzitic sands, and the water−xenon−hydrate interface is inferred to relax water molecules more quickly than the water−quartzitic−sand interface. The value of NMR ρ 2 changes when gas hydrate is of grain-coating, pore-filling, or graintouching habit, and predictions of hydraulic permeabilities and water retention curves based on NMR T 2 spectra need to be modified under this condition. However, patchy hydrate widespread in natural coarse-grained sediments has little effect on the value of NMR ρ 2 , and there is no need of significant modifications for hydraulic permeability and water retention curve predictions. This study has a great potential to further hydrate related NMR applications both in artificial and natural environments.