The Bamboo species accounts for almost 1% of the Earth’s forested area with an exceptionally fast growth peaking up to 7.5–100 cm per day during the growing period, making it an unique species with respect to measuring and monitoring using conventional forest inventory tools. In addition their widespread coverage and quick growth make them a critical component of the terrestrial carbon cycle and for mitigating the impacts of climate change. In this study, the capability of using airborne Light Detection and Ranging (LiDAR) data for estimating canopy structure and biomass of Moso bamboo (Phyllostachys pubescens) was assessed, which is one of the most valuable and widely distributed bamboo species in the subtropical forests of south China. To do so, we first evaluated the accuracy of using LiDAR data to interpolate the underlying ground terrain under bamboo forests and developed uncertainty surfaces using both LiDAR-derived vegetation and topographic metrics and a Random Forest (RF) classifier. Second, we utilized Principal Component Analysis (PCA) to quantify the variation of the vertical distribution of LiDAR-derived effective Leaf Area Index (LAI) of bamboo stands, and fitted regression models between selected LiDAR metrics and the field-measured attributes such mean height, DBH and biomass components (i.e., culm, branch, foliage and aboveground biomass (AGB)) across a range of management strategies. Once models were developed, the results were spatially extrapolated and compared across the bamboo stands. Results indicated that the LiDAR interpolated DTMs were accurate even under the dense intensively managed bamboo stands (RMSE = 0.117–0.126 m) as well as under secondary stands (RMSE = 0.102 m) with rugged terrain and near-ground dense vegetation. The development of uncertainty maps of terrain was valuable when examining the magnitude and spatial distribution of potential errors in the DTMs. The middle height intervals (i.e., HI4 and HI5) within the bamboo cumulative effective LAI profiles explained more variances by PCA analysis in the bamboo stands. Moso bamboo AGB was well predicted by the LiDAR metrics (R2 = 0.59–0.87, rRMSE = 11.92–21.11%) with percentile heights (h25-h95) and the coefficient of variation of height (hcv) having the highest relative importances for estimating AGB and culm biomass. The hcv explained the most variance in branch and foliage biomass. According to the spatial extrapolation results, areas of relatively low biomass were found on secondary stands (AGB = 49.42 ± 14.16 Mg ha−1), whereas the intensively managed stands (AGB = 173.47 ± 34.16 Mg ha−1) have much higher AGB and biomass components, followed by the extensively managed bamboo stands (AGB = 67.61 ± 13.10 Mg ha−1). This study demonstrated the potential benefits of using airborne LiDAR to accurately derive high resolution DTMs, characterize vertical structure of canopy and estimate the magnitude and distribution of biomass within Moso bamboo forests, providing key data for regional ecological, environmental and global carbon cycle models.