To date, Bi 2 Se 3 is known as the best three-dimensional high temperature topological insulator with a large bulk band gap. Here, we theoretically predict that the series of Pb-based layered chalcogenides, Pb n Bi 2 Se n+3 and Pb n Sb 2 Te n+3 , are possible new candidates for topological insulators. As n increases, the phase transition from a topological insulator to a band insulator is found to occur between n = 2 and 3 for both series. Significantly, among the new topological insulators, we found a bulk band gap of 0.40eV in PbBi 2 Se 4 which is one of the largest gap topological insulators, and that Pb 2 Sb 2 Te 5 is located in the immediate vicinity of the topological phase boundary, making its topological phase easily tunable by changing external parameters such as lattice constants. Due to the three-dimensional Dirac cone at the phase boundary, massless Dirac fermions also may be easily accessible in Pb 2 Sb 2 Te 5 .