In this paper, we employ the theory of Lagrangian coherent structures for three-dimensional vortex eduction and investigate the effect of large-scale vortical structures on the turbulent/non-turbulent interface (TNTI) and entrainment of a gravity current. The gravity current is realized experimentally and different levels of stratification are examined. For flow measurements, we use a multivolume three-dimensional particle tracking velocimetry technique. To identify vortical Lagrangian coherent structures (VLCSs), a fully automated three-dimensional extraction algorithm for multiple flow structures based on the so-called Lagrangian-averaged vorticity deviation method is implemented. The size, the orientation and the shape of the VLCSs are analysed and the results show that these characteristics depend only weakly on the strength of the stratification. Through conditional analysis, we provide evidence that VLCSs modulate the average TNTI height, consequently affecting the entrainment process. Furthermore, VLCSs influence the local entrainment velocity and organize the flow field on both the turbulent and non-turbulent sides of the gravity current boundary.