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The aim of the current study was to investigate the feasibility of three‐dimensional ultrashort echo time quantitative susceptibility mapping (3D UTE‐QSM) for the assessment of gadolinium (Gd) deposition in cortical bone. To this end, 40 tibial bovine cortical bone specimens were divided into five groups then soaked in phosphate‐buffered saline (PBS) solutions with five different Gd concentrations of 0, 0.4, 0.8, 1.2, and 1.6 mmol/L for 48 h. Additionally, eight rabbits were randomly allocated into three groups, consisting of a normal‐dose macrocyclic gadolinium‐based contrast agent (GBCA) group (n = 3), a high‐dose macrocyclic GBCA group (n = 3), and a control group (n = 2). All bovine and rabbit tibial bone samples underwent magnetic resonance imaging (MRI) on a 3‐T clinical MR system. A 3D UTE‐Cones sequence was utilized to acquire images with five different echo times (i.e., 0.032, 0.2, 0.4, 0.8, and 1.2 ms). The UTE images were subsequently processed with the morphology‐enabled dipole inversion algorithm to yield a susceptibility map. The average susceptibility was calculated in three regions of interest in the middle of each specimen, and the Pearson's correlation between the estimated susceptibility and Gd concentration was calculated. The bone samples soaked in PBS with higher Gd concentrations exhibited elevated susceptibility values. A mean susceptibility value of −2.47 ± 0.23 ppm was observed for bovine bone soaked in regular PBS, while the mean QSM value increased to −1.75 ± 0.24 ppm for bone soaked in PBS with the highest Gd concentration of 1.6 mmol/L. A strong positive correlation was observed between Gd concentrations and QSM values. The mean susceptibility values of rabbit tibial specimens in the control group, normal‐dose GBCA group, and high‐dose GBCA group were −4.11 ± 1.52, −3.85 ± 1.33, and −3.39 ± 1.35 ppm, respectively. In conclusion, a significant linear correlation between Gd in cortical bone and QSM values was observed. The preliminary results suggest that 3D UTE‐QSM may provide sensitive noninvasive assessment of Gd deposition in cortical bone. [ABSTRACT FROM AUTHOR]