The living vegetation volume (LVV) can accurately describe the spatial structure of greening trees and quantitatively represent the relationship between this greening and its environment. Because of the mostly line shape distribution and the complex species of street trees, as well as interference from artificial objects, current LVV survey methods are normally limited in their efficiency and accuracy. In this study, we propose an improved methodology based on vehicle-mounted LiDAR data to estimate the LVV of urban street trees. First, a point-cloud-based CSP (comparative shortest-path) algorithm was used to segment the individual tree point clouds, and an artificial objects and low shrubs identification algorithm was developed to extract the street trees. Second, a DBSCAN (density-based spatial clustering of applications with noise) algorithm was utilized to remove the branch point clouds, and a bottom-up slicing method combined with the random sampling consistency iterative method algorithm (RANSAC) was employed to calculate the diameters of the tree trunks and obtain the canopy by comparing the variation in trunk diameters in the vertical direction. Finally, an envelope was fitted to the canopy point cloud using the adaptive AlphaShape algorithm to calculate the LVVs and their ecological benefits (e.g., O2 production and CO2 absorption). The results show that the CSP algorithm had a relatively high overall accuracy in segmenting individual trees (overall accuracy = 95.8%). The accuracies of the tree height and DBH extraction based on vehicle-mounted LiDAR point clouds were 1.66~3.92% (rRMSE) and 4.23~15.37% (rRMSE), respectively. For the plots on Zijin Mountain, the LVV contribution by the maple poplar was the highest (1049.667 m3), followed by the sycamore tree species (557.907 m3), and privet’s was the lowest (16.681 m3).