PURPOSE:To investigate quantitative 2D ultrashort echo time magnetization transfer (UTE-MT) imaging in ex vivo bovine cortical bone and in vivo human tibial cortical bone. METHODS:Data were acquired from five fresh bovine cortical bone samples and five healthy volunteer tibial cortical bones using a 2D UTE-MT sequence on a clinical 3T scanner. The 2D UTE-MT sequence used four or five MT powers with five frequency offsets. Results were analyzed with a two-pool quantitative MT model, providing measurements of macromolecular fraction (f), macromolecular proton transverse relaxation times (T2m ), proton exchange rates from water/macromolecular to the macromolecular/water pool (RM0m /RM0w ), and spin-lattice relaxation rate of water pool (R1w ). A sequential air-drying study for a small bovine cortical bone chip was used to investigate whether above MT modeling parameters were sensitive to the water loss. RESULTS:Mean fresh bovine cortical bone values for f, T2m , R1w , RM0m , and RM0w were 59.9 ± 7.3%, 14.6 ± 0.3 μs, 9.9 ± 2.4 s-1 , 17.9 ± 3.6 s-1 , and 11.8 ± 2.0 s-1 , respectively. Mean in vivo human cortical bone values for f, T2m , R1w , RM0m and RM0w were 54.5 ± 4.9%, 15.4 ± 0.6 μs, 8.9 ± 1.1 s-1 , 11.5 ± 3.5 s-1 , and 9.5 ± 1.9 s-1 , respectively. The sequential air-drying study shows that f, RM0m , and R1w were increased with longer drying time. CONCLUSION:UTE-MT two-pool modeling provides novel and useful quantitative information for cortical bone. Magn Reson Med 79:1941-1949, 2018. © 2017 International Society for Magnetic Resonance in Medicine.