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Urban forest carbon sequestration represents an important component of the global forest carbon pool; however, accurate measurements are limited by the inability of existing field stand models to match the specificity of urban greening species. Herein, canopy volume, carbon stock, and the biomass expansion factor (BEF) of 30 <i>Koelreuteria paniculate</i> trees were measured based on terrestrial laser scanning (TLS) and compared to the results of existing wood volume and carbon stock model measurements. The findings revealed that (1) TLS point cloud data were highly reproducible and accurate (root mean square error of tree height and diameter at breast height were ±0.35 m and ±0.33 cm, respectively). (2) Owing to human interference and cluttered urban environments, the BEF of urban greening tree species fluctuated irregularly, considerably different from that of natural forest stands. (3) Leaf carbon stocks were influenced by the size of the voxel. (4) Different tree measurement factors maintained variable degrees of influence on BEF (height under branch, volume of thick branch, crown width, and projected areas of tree-crown produced correlation coefficients of −0.64, 0.54, 0.45, and 0.43, respectively). Accordingly, the carbon stock and BEF of urban greening tree species can be accurately calculated via TLS without damage.