This study investigates the imaging ability of the time-domain linear sampling method (TLSM) when applied to laser ultrasonic (LU) tomography of subsurface defects from limited-aperture measurements. In this vein, the TLSM indicator and it spectral counterpart known as the multifrequency LSM are formulated within the context of LU testing. The affiliated imaging functionals are then computed using synthetic and experimental data germane to LU inspection of aluminum alloy specimens with manufactured defects. Hyperparameters of inversion are computationally analyzed. We demonstrate using synthetic data that the TLSM indicator has the unique ability to recover weak (or hard-to-reach) scatterers and has the potential to generate higher quality images compared to LSM. Provided high-SNR measurements, this advantage may be preserved in reconstructions from LU test data.