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Crown vertical profiles (CVP) play an essential role in stand biomass and forest fire prediction. Traditionally, due to measurement difficulties, CVP models developed based on a small number of individual trees are not convincing. Terrestrial laser scanning (TLS) provides new insights for researching trees' CVPs. However, there is a limited understanding of the ability to accurately describe CVPs with TLS. In this study, we propose a new approach to automatically extract the crown radius (CR) at different heights and confirm the correctness and effectiveness of the proposed approach with field measurement data from 30 destructively harvested sample trees. We then applied the approach to extract the CR from 283 trees in 6 sample plots to develop a two-level nonlinear mixed-effects (NLME) model for the CVP. The results of the study showed that the average extraction accuracy of the CR when the proposed approach was applied was 90.12%, with differences in the extraction accuracies at different relative depths into the crown (RDINC) ranges. The TLS-based extracted CR strongly correlated with the field-measured CR, with an R2 of 0.93. Compared with the base model, the two-level NLME model has significantly improved the prediction accuracy, with Ra2 increasing by 13.8% and RMSE decreasing by 23.46%. All our research has demonstrated that TLS has great potential for accurately extracting CRs, which would provide a novel way to nondestructively measure the crown structure. Moreover, our research lays the foundation for the future development of CVP models using TLS at a regional scale. [ABSTRACT FROM AUTHOR]