PurposeTo develop and assess a new technique for three‐dimensional (3D) full lung T1 and T2* mapping using a single free breathing scan during a clinically feasible time.Materials and MethodsA 3D stack of dual‐echo ultrashort echo time (UTE) radial acquisition interleaved with and without a WET (water suppression enhanced through T1 effects) saturation pulse was used to map T1 and T2* simultaneously in a single scan. Correction for modulation due to multiple views per segment was derived. Bloch simulations were performed to study saturation pulse excitation profile on lung tissue. Optimization of the saturation delay time (for T1 mapping) and echo time (for T2* mapping) was performed. Monte Carlo simulation was done to predict accuracy and precision of the sequence with signal‐to‐noise ratio of in vivo images used in the simulation. A phantom study was carried out using the 3D interleaved saturation recovery with dual echo ultrashort echo time imaging (ITSR‐DUTE) sequence and reference standard inversion recovery spin echo sequence (IR‐SE) to compare accuracy of the sequence. Nine healthy volunteers were imaged and mean (SD) of T1 and T2* in lung parenchyma at 3T were estimated through manually assisted segmentation. 3D lung coverage with a resolution of 2.5 × 2.5 × 6 mm3 was performed and nominal scan time was recorded for the scans. Repeatability was assessed in three of the volunteers. Regional differences in T1/T2* values were also assessed.ResultsThe phantom study showed accuracy of T1 values to be within 2.3% of values obtained from IR‐SE. Mean T1 value in lung parenchyma was 1002 ± 82 ms while T2* was 0.85 ± 0.1 ms. Scan time was ∼10 min for volunteer scans. Mean coefficient of variation (CV) across slices was 0.057 and 0.09, respectively. Regional variation along the gravitational direction and between right and left lung were not significant (P = 0.25 and P = 0.06, respectively) for T1. T2* showed significant variation (P = 0.03) along the gravitational direction. Repeatability for three volunteers was within 0.7% for T1 and 1.9% for T2*.Conclusion3D T1 and T2* maps of the entire lung can be obtained in a single scan of ∼10 min with a resolution of 2.5 × 2.5 × 6 mm3.Level of Evidence: 2J. Magn. Reson. Imaging 2017;45:1097–1104