Grey Herons (Ardea cinerea) typically prey upon fish and other aquatic organisms with occasional reports of predating small birds. I report observations of one or more Grey Herons predating on Aldabra White-throated Rails (Dryolimnas cuvieri aldabranus) on Picard Island (Aldabra Atoll, Seychelles). Grey Herons were observed on two occasions having caught rails and, on another occasion, a heron was observed ambushing and pursuing rails with no success. Heron(s) were not observed ingesting the rails, as they flew or ran off with their prey, but it is likely the rails were consumed. These are the first observations of any form of predation on the Aldabra White-throated Rail, which is one of the largest recorded avian prey of the Grey Heron.