We report a systematic angle-resolved photoemission spectroscopy on topological insulator (TI) TlBi1−xSbxTe2 which is bulk insulating at 0.5 x 0.9 and undergoes a metal-insulator-metal transition with the Sb content x. We found that this transition is characterized by a systematic hole doping with increasing x, which results in the Fermi-level crossings of the bulk conduction and valence bands at x ∼ 0 and x ∼ 1, respectively. The Dirac point of the topological surface state is gradually isolated from the valence-band edge, accompanied by a sign reversal of Dirac carriers. We also found that the Dirac velocity is the largest among known solid-solution TI systems. The TlBi1−xSbxTe2 system thus provides an excellent platform for Dirac-cone engineering and device applications of TIs. The three-dimensional topological insulator (3D TI) is a novel quantum state of matter with a metallic surface state and an insulating bulk. The surface state is characterized by linearly dispersive Dirac-cone band dispersion which traverses the bulk-band gap generated by the spin-orbit coupling [1][2][3]. Experimental realization of various exotic topological phenomena, such as the topological magnetoelectric effect and anomalous quantum Hall effect, [4][5][6] as well as the device applications of TIs largely rely on the dominance of surface Dirac transport and the capability to manipulate Dirac-carrier properties, whereas it is difficult to achieve highly insulating bulk in most of known the 3D TIs due primarily to the small bulk-band gap and defects in the crystal.One of the promising strategies to achieve insulating bulk is to reduce defects [7,8] and compensate defect-induced carriers by tuning chemical composition in a solid-solution system. This methodology has been successfully applied to bulk crystals of tetradymite Bi 2−x Sb x Te 3−y Se y (BSTS) where special combinations of x and y yield high resistivity [9][10][11][12]. Angle-resolved photoemission spectroscopy (ARPES) study of BSTS has revealed a sign reversal of Dirac carriers while keeping insulating bulk [13]. Discovery of the BSTS system has accelerated the engineering of Dirac carriers and device applications [11,[14][15][16][17][18][19][20][21], as highlighted by the spin injection via spin-pumping technique [17], electrical detection of spin polarization [18], and realization of quantum Hall effect at high temperature [19]. To further realize exotic quantum phenomena and device applications in TIs, it is of particular importance to explore the new materials platform of bulk-insulating TIs, since the essential characteristics of bulk and surface, such as the bulk-band gap and the Dirac velocity, strongly depend on the material.Rhombohedral III-V-VI 2 ternary chalcogenide TlM'X 2 [M = Bi and Sb; X = S, Se, and Te; see Figs. 1(a) and 1(b) for the crystal structure and Brillouin zone (BZ), respectively] [22-26] is an intriguing platform to achieve insulating TIs since its crystal structure is distinct from tetradymite due to the covalent-bonding nature and the absence o...