The understory is an essential ecological and structural component of forest ecosystems. The lack of efficient, accurate, and objective methods for evaluating and quantifying the spatial spread of understory characteristics over large areas is a challenge for forest planning and management, with specific regard to biodiversity and habitat governance. In this study, we used terrestrial and airborne laser scanning (TLS and ALS) data to characterize understory in a European beech and black pine forest in Italy. First, we linked understory structural features derived from traditional field measurements with TLS metrics, then, we related such metrics to the ones derived from ALS. Results indicate that (i) the upper understory density (5–10 m above ground) is significantly associated with two ALS metrics, specifically the mean height of points belonging to the lower third of the ALS point cloud within the voxel (HM1/3) and the corresponding standard deviation (SD1/3), while (ii) for the lower understory layer (2–5 m above ground), the most related metric is HM1/3 alone. As an example application, we have produced a map of forest understory for each layer, extending over the entire study region covered by ALS data, based on the developed spatial prediction models. With this study, we also demonstrated the power of hand-held mobile-TLS as a fast and high-resolution tool for measuring forest structural attributes and obtaining relevant ecological data.