This paper investigates the Vander Waals heterostructure of organic rubrene and topological insulator Bi2Se3 with an atomically abrupt interface with exciting applications in electronic and optoelectronic devices. This organic/inorganic heterostructure (OIH) was prepared using a simple two-step physical vapor deposition process; based on this hybrid structure, a self-powered photodetector was then constructed. The Dirac surface state at the heterointerface enhances the splitting and transferring of photo-generated carriers, resulting in improved device characteristics. Under 1064 nm, the prepared photodetectors demonstrated a maximum responsivity (6.37 A/W), a high detectivity (3.42 × 1010 Jones), and ultrafast photoresponse speeds with rise time (1.17 µs) and decay time (1.59 µs), respectively. These promising results suggest that these PDs can be used in various photodetection applications and may lead to developing new devices.