Printable and flexible organic phototransistors (OPTs) make comprehensive requirements for the organic semiconductors (OSCs), including high photosensitivity, decent transistor characteristics, appropriate solution viscosity, and good film flexibility. It has been challenging to obtain such semiconductors. Here, we demonstrated that by taking advantage of the interfacial charge effect, printable and flexible OPTs with high performance can be successfully fabricated through simply blending common OSCs with polymers. Using 2,7‐dioctyl[1]benzothieno[3,2‐b][1]benzothiophene and an insulating biopolymer polylactide, OPTs with blended and layered structure are both fabricated and investigated. The photoresponses of the OPTs can be modulated by gate voltage over 1000 times, and their responsivities are measured up to 400 A W−1. As compared to the layered OPTs, the blended ones exhibit higher photocurrent to dark current ratio (up to 105) and better light detection limit (lower than 0.02 mW cm−2). The improvements are attributed to larger interfacial area and more intensive charge trapping effect. The flexible OPTs are further fabricated by inkjet printing the blended solution. This work presents OPTs with comprehensive advantages including low cost, enhanced photosensitivity, great flexibility, and printability, which are realized by simply blending common OSC with polymer, and thus provide an inspiration for the design of novel organic electronics.

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