A criterion for identifying vortex ring pinch-off based on the Lagrangian coherent structures ͑LCSs͒ in the flow is proposed and demonstrated for a piston-cylinder arrangement with a piston stroke to diameter ͑L / D͒ ratio of Ϸ12. It is found that the appearance of a new disconnected LCS and the termination of the original LCS are indicative of the initiation of vortex pinch-off. The subsequent growth of new LCSs, which tend to roll into spirals, indicates the formation of new vortex cores in the trailing shear layer. Using this criterion, the formation number is found to be 4.1Ϯ 0.1, which is consistent with the predicted formation number of Ϸ4 of Gharib et al. ͓J. Fluid Mech. 360, 121 ͑1998͔͒. The results obtained using the proposed LCS criterion are compared with those obtained using the circulation criterion of Gharib et al. and are found to be in excellent agreement. The LCS approach is also compared against other metrics, both Lagrangian and Eulerian, and is found to yield insight into the pinch-off process that these do not. Furthermore, the LCS analysis reveals a consistent pattern of coalescing or "pairing" of adjacent vortices in the trailing shear layer, a process which has been extensively documented in circular jets. Given that LCSs are objective and insensitive to local errors in the velocity field, the proposed criterion has the potential to be a robust tool for pinch-off identification. In particular, it may prove useful in the study of unsteady and low Reynolds number flows, where conventional methods based on vorticity prove difficult to use. © 2010 American Institute of Physics. ͓doi:10.1063/1.3275499͔The formation of axisymmetric vortex rings is a widely occurring phenomenon both in nature and in industry. It is known that these vortex rings cannot grow indefinitely, but rather there is a physical limit to their size.1 Beyond this limit, vortex rings do not grow any further but "pinch off," and a trailing jet forms behind them. This limit implies the existence of an optimum vortex size: for optimum momentum transfer, rings must be made as large as possible while avoiding pinch-off.2 This optimum has important implications for natural and engineering flows, and hence vortex ring pinch-off has been extensively studied, principally by means of the vorticity field. However, in the more complex naturally occurring flows, the vorticity field tends to break down and diffuse, and existing criteria prove insufficient for robustly identifying pinch-off. In this paper we propose a criterion for pinchoff identification, based on Lagrangian coherent structures (LCSs), which could provide further insight into the structure of these complex natural flows. The criterion is demonstrated for a laboratory-generated vortex ring, and it is found to be in good agreement with the established criterion based on circulation.