The spectral clustering method has notable advantages in segmentation. But the high computational complexity and time consuming limit its application in large-scale and dense airborne Light Detection and Ranging (LiDAR) point cloud data. We proposed the Nyström-based spectral clustering (NSC) algorithm to decrease the computational burden. This novel NSC method showed accurate and rapid in individual tree segmentation using point cloud data. The K-nearest neighbour-based sampling (KNNS) was proposed for the Nyström approximation of voxels to improve the efficiency. The NSC algorithm showed good performance for 32 plots in China and Europe. The overall matching rate and extraction rate of proposed algorithm reached 69% and 103%. For all trees located by Global Navigation Satellite System (GNSS) calibrated tape-measures, the tree height regression of the matching results showed an value of 0.88 and a relative root mean square error (RMSE) of 5.97%. For all trees located by GNSS calibrated total-station measures, the values were 0.89 and 4.49%. The method also showed good performance in a benchmark dataset with an improvement of 7% for the average matching rate. The results demonstrate that the proposed NSC algorithm provides an accurate individual tree segmentation and parameter estimation using airborne LiDAR point cloud data.