Forest canopies exert significant controls over the spatial distribution of snow cover. Canopy snow interception efficiency is controlled by intrinsic processes (e.g., canopy structure), extrinsic processes (e.g., meteorological conditions), and the interaction of intrinsic-extrinsic factors (i.e., air temperature and branch stiffness). In hydrological models, intrinsic processes governing snow interception are typically represented by two-dimensional metrics like the leaf area index (LAI). To improve snow interception estimates and their scalability, new approaches are needed for better characterizing the three-dimensional distribution of canopy elements. Airborne laser scanning (ALS) provides a potential means of achieving this, with recent research focused on using ALS-derived metrics that describe forest spacing to predict interception storage. A wide range of canopy structural metrics that describe individual trees can also be extracted from ALS, although relatively little is known about which of them, and in what combination, best describes intrinsic canopy properties known to affect snow interception. The overarching goal of this study was to identify important ALS-derived canopy structural metrics that could help to further improve our ability to characterize intrinsic factors affecting snow interception. Specifically, we sought to determine how much variance in canopy intercepted snow volume can be explained by ALS-derived crown metrics, and what suite of existing and novel crown metrics most strongly affects canopy intercepted snow volume. To achieve this, we first used terrestrial laser scanning (TLS) to quantify snow interception on 14 trees. We then used these snow interception measurements to fit a random forest model with ALS-derived crown metrics as predictors. Next, we bootstrapped 1000 calculations of variable importance (percent increase in mean squared error when a given explanatory variable is removed), keeping nine canopy metrics for the final model that exceeded a variable importance threshold of 0.2. ALS-derived canopy metrics describing intrinsic tree structure explained approximately two-thirds of the snow interception variability (R2 ≥ 0.65, RMSE ≤ 0.52 m3, relative RMSE ≤ 48%) in our study when extrinsic factors were kept as constant as possible. For comparison, a generalized linear mixed-effects model predicting snow interception volume from LAI alone had a marginal R2 = 0.01. The three most important predictor variables were canopy length, whole-tree volume, and unobstructed returns (a novel metric). These results suggest that a suite of intrinsic variables may be used to map interception potential across larger areas and provide an improvement to interception estimates based on LAI.