Precise delineation of individual tree crowns is critical for accurate forest biophysical parameter estimation, species classification, and ecosystem modelling. Multispectral optical remote sensors mounted on low-flying unmanned aerial vehicles (UAVs) can rapidly collect very-high-resolution (VHR) photogrammetric optical data that contain the spectral, spatial, and structural information of trees. State-of-the-art tree crown delineation approaches rely mostly on spectral information and un-derexploit the spatial-contextual and structural information in VHR photogrammetric multispectral data, resulting in crown delineation errors. Here, we propose the spectral, spatial-contextual, and structural information-based individual tree crown delineation (S3-ITD) method, which accurately delineates individual spruce crowns by minimizing the undesirable effects due to intracrown spectral variance and nonuniform illumination/shadowing in VHR multispectral data. We evaluate the performance of the S3-ITD crown delineation method over a white spruce forest in Quebec, Canada. The highest mean intersection over union (IoU) index of 0.83, and the lowest mean crown-area difference (CAD) of 0.14 m², proves the superior crown delineation performance of the S3-ITD method over state-of-the-art methods. The reduction in error by 2.4 cm and 1.0 cm for the allometrically derived diameter at breast height (DBH) estimates compared with those from the WS-ITD and the BF-ITD approaches, respectively, demonstrates the effectiveness of the S3-ITD method to accurately estimate biophysical parameters.