Airborne light detection and ranging (LiDAR) data are increasingly used to inform sustainable forest management practices. Information about species composition is needed for a range of applications; however, commonly used area-based summaries of LiDAR data are limited to accurately differentiate tree species. The objective of this study was to map dominant species groups across a large (>580,000 ha) boreal forest by combining area-based and individual tree metrics derived from single photon LiDAR data with multispectral information derived from Sentinel-2 imagery. Classification of the forest into jack pine (Pinus banksiana), black spruce (Picea mariana), mixed conifer, mixedwood, and hardwood species groups resulted in an overall accuracy of 67.8% compared with field data. A more generalized classification into softwood, hardwood, and mixedwood had an overall accuracy of 83.2%. The reflectance in the red edge region of the electromagnetic spectrum (λ = 740 nm), the area and volume of tree crowns, and the cumulative distribution of LiDAR returns in the canopy were particularly important variables to discriminate between species groups. Wall-to-wall predictions of species groups based on remotely sensed data—as derived herein—could provide a spatially-detailed alternative to stand-level species composition information traditionally derived from photo-interpreted aerial imagery.