Filter-free band-selective photodetectors with tunable band edges possess extensive applications in smart sensors, artificial intelligence, the internet of everything, and so forth. However, such photodetectors operated with the charge collection narrowing effect require a thick active layer over millimeters, leading to rather a large device size, high material cost, and limited mechanical flexibility. In this work, we report a flexible thin-film perovskite and organic semiconductor (OSC) heterojunction device, which can achieve adjustable band-selective photodetection by utilizing the easy tunability of the perovskite band gap. First, heterojunction photodiodes with only two active layers of perovskites and OSCs are fabricated, in which the perovskite contributes to light absorption and rectification characteristics simultaneously. The fundamental device operation mechanism is investigated by combining the band alignments of the heterojunctions and their potential distributions observed with Kelvin probe force microscopy. It uncovers that the presence of built-in electric fields in the heterojunctions caused by moderate band alignments and appropriate difference in hole and electron concentrations between the perovskites and the OSCs is significant for the properties of the photodiodes. The resultant photodiodes exhibit a high rectification ratio of up to 10 3 , decent photodetection performance, and mechanical flexibility. Furthermore, photodetectors based on perovskite/OSC/perovskite stack heterojunctions can realize the functions of filterless band-selective photodetection in a single device, and the band edges in the photodetection can be modulated by tuning the perovskite band gap. Therefore, this work provides flexible thin-film photodiodes with the potential of miniaturization and low-cost fabrication and demonstrates tunable band-selective photodetection for advanced applications.