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IPv4 and IPv6 will coexist for many years during the transition period from the traditional IPv4-based Internet to an IPv6-based Internet. DHTLayer, a novel IPv4/IPv6 transition mechanism based on Distributed Hash Table (DHT) is presented in this paper. It can fully support IPv4 and IPv6 inter-operation. DHTLayer employs a DHT overlay to maintain the routing information between IPv4 and IPv6. It decouples path selection from packet delivery. In DHTLayer, the Looking-Up Route Path is responsible for selecting paths, and then the Delivering Process takes charge of delivering IP packets along the path selected above. Simulation results show that it is very effective and efficient.