Carrier scattering in photodetectors employing 2D dichalcogenide as an absorber impedes carrier transport. As scattering at the interface between the semiconductor and the electrode restricts carrier transport, it is essential to develop alternative electrode materials to achieve high photoresponsivity. A carrier can effectively move through a topologically protected Dirac surface state without scattering: i.e., alternatives such as topological insulators (TI) containing the surface state can effectively reduce scattering at the interface between the semiconductor and the electrode. In this stucy, TI Bi2Se3 with a well-ordered interfacial structure was used as a carrier transport layer (CTL) to effectively employ the topological surface state (TSS) for improving WSe2 photoresponsivity. At 520 nm, the Bi2Se3 TI-CTL photodetector has a photoresponsivity of up to 11.47 AW−1, 100 times higher than the photodevice using only Au electrodes. The photoresponsivity and time-resolved photoluminescence as a function of thickness indicate that TSS contributes to improved carrier separation with high carrier transfer efficiency, thereby affecting photocurrent generation. The fast carrier transfer through TSS helps efficiently separate electron-hole pairs and suppress recombination at the interface, generating ultra-fast and high-efficiency photocurrents in the broadband region (450–1550 nm). Therefore, TSS based on carrier dynamics can lead to further applications of next-generation optoelectronic devices.