Unsupervised segmentation of Terrestrial Laser Scanning (TLS) data into wood and leaf is the key for studying forest carbon storage, photosynthesis, canopy radiation. Further segmentation of wood data into trunk and larger branch (TLB), remaining branch (RB) is of great significance and challenge for dust retention, soil heavy metal enrichment. We proposed an unsupervised, automatic semantic segmentation method based on TLS data of individual tree. The method firstly performs initial segmentation based on plane fitting residuals and neighborhood normal angle, which can extract smooth and connected regions in point cloud. Then, the geometric features of segmented clusters are quantified to approximate RB or leaf features. Finally, the segmentation of TLB, RB, and leaf is realized by combining different clusters from bottom to top with geometric features and neighborhood relations. The segmentation performance of our method was evaluated with 104 tree samples from 23 tree species in two open-source datasets from Indonesia, Peru, Guyana and from Canada and Finland. The micro-average precision of our method is 93.61%. The micro-average recalls of TLB, RB, and leaf are 97.08%, 86.44%, and 89.62%. Compared with the well-known method of separating wood and leaf, our method has 33.56% higher sensitivity, 1.82% higher specificity, 20.52% higher precision, and 0.217 higher F1-score. Besides, we estimated the surface area and volume of TLB, the surface area and volume of RB based on the segmented data. The above parameters have good consistency compared to those calculated based on manually separated point clouds (Pearson correlation coefficient (PCC) of 0.55-0.93).