We report a comprehensive high-pressure study on the monoclinic TlFeSe2 single crystal, which is an antiferromagnetic insulator with quasi-one-dimensional crystal structure at ambient pressure. It is found that TlFeSe2 undergoes a pressure-induced structural transformation from the monoclinic phase to an orthorhombic structure above P
c ≈ 13 GPa, accompanied with a large volume collapse of ΔV/V
0 = 8.3%. In the low-pressure monoclinic phase, the insulating state is easily metallized at pressures above 2 GPa; while possible superconductivity with
T
c
onset
∼
2
K is found to emerge above 30 GPa in the high-pressure phase. Such a great tunability of TlFeSe2 under pressure indicates that the ternary AFeSe2 system (A = Tl, K, Cs, Rb) should be taken as an important platform for explorations of interesting phenomena such as insulator-metal transition, dimensionality crossover, and superconductivity.