Forest understory vegetation is an important characteristic of the forest. Predicting and mapping understory is a critical need for forest management and conservation planning, but it has proved difficult with available methods to date. LiDAR has the potential to generate remotely sensed forest understory structure data, but this potential has yet to be fully validated. Our objective was to examine the capacity of LiDAR point cloud data to predict forest understory cover. We modeled ground-based observations of understory structure in three vertical strata (0.5 m to < 1.5 m, 1.5 m to < 2.5 m, 2.5 m to < 3.5 m) as a function of a variety of LiDAR metrics using both mixed-effects and Random Forest models. We compared four understory LiDAR metrics designed to control for the spatial heterogeneity of sampling density. The four metrics were highly correlated and they all produced high values of variance explained in mixed-effects models. The top-ranked model used a voxel-based understory metric along with vertical stratum (Akaike weight = 1, explained variance = 87%, cross-validation error = 15.6%). We found evidence of occlusion of LiDAR pulses in the lowest stratum but no evidence that the occlusion influenced the predictability of understory structure. The Random Forest model results were consistent with those of the mixed-effects models, in that all four understory LiDAR metrics were identified as important, along with vertical stratum. The Random Forest model explained 74.4% of the variance, but had a lower cross-validation error of 12.9%. We conclude that the best approach to predict understory structure is using the mixed-effects model with the voxel-based understory LiDAR metric along with vertical stratum, because it yielded the highest explained variance with the fewest number of variables. However, results show that other understory LiDAR metrics (fractional cover, normalized cover and leaf area density) would still be effective in mixed-effects and Random Forest modelling approaches.