Light detection and ranging (LiDAR) has been widely used to estimate forest biomass. In this study, we aim to further explore this capability by correlating horizontal and vertical distribution of LiDAR data with components of biomass in a Picea crassifolia forest. Airborne small footprint full-waveform data were decomposed to acquire higher density point clouds. We calculated LiDAR metrics at the tree level and subplot level and correlated them to biomass components, including branch biomass (BB), leaf biomass (LB) and above-ground biomass (AGB), respectively. A new metric (Horizcv) describing the horizontal distribution of point clouds was proposed. This metric was found to be highly correlated with canopy biomass (BB and LB) at the tree level and subplot level. Correlation between AGB and Horizcv at the subplot level is much lower than that at tree level. AGB for subplot is highly correlated with the mean height metric (Hmean), canopy cover index (CCI) and the product of them. On the other hand, the relationship between the vertical distribution of LiDAR point and biomass was explored by developing two types of vertical profiles, including LiDAR distribution profiles and a biomass profile. Good relationships were found between these two types of vertical profiles and assessed by Pearson’s correlation coefficient (R) and the area of overlap index (AOI). These good correlations possess potential in predicting the vertical distribution of canopy biomass. Overall, it is concluded that not only the vertical, but also the horizontal distribution of LiDAR points should be taken into account in estimating components of biomass by LiDAR.