The lack of time resolution restricts the quantitative detection of shallow subsurface defects with ultrasonic time-of-flight diffraction (TOFD) technique due to the superposition between lateral wave and diffracted waves from upper and lower tips. In this article, the frequency-domain sparsity-decomposability inversion (FDSDI) method was proposed to enhance the time resolution in TOFD based on the sparsity and decomposability of the ultrasonic reflection sequence. An optimization problem was formulated in the frequency domain by combining l1 - and l2 -norm constraints. The simulation was performed with a carbon steel model containing a series of shallow subsurface cracks at the depths of 2.0, 2.5, 3.0, 3.5, and 4.0 mm. The relative measurement errors of defect depths and heights were no more than 6.57%, and the depth of the dead zone was reduced by 70%. Subsequently, the feasibility of the FDSDI method was experimentally verified on a carbon steel specimen with an artificial defect. The defect depth and height were calculated with relative errors within 6.0%. Finally, the detection capacity of the FDSDI method was discussed, and the effects of frequency bandwidth, regularization parameter, and noise on inversion results were analyzed by experiments. It is concluded that the FDSDI method decouples the multiple overlapped signals and significantly improves the time resolution to quantify the small defects in the dead zone.