Br, I) have attracted much attention due to their superior photoelectric properties, for example, direct band gap (≈1.6 eV), small exciton binding energy (≈20 meV), broad absorption range, long-range exciton diffusion length (100-1000 nm). [7][8][9] Thus they play as important candidates in the field of renewable photovoltaic or photoelectric devices. [10][11][12][13] Perovskite materials were introduced into solar cells in 2009 with the power conversion efficiencies (PCEs) of about 3.81%, and the PCEs of state-ofthe-art perovskite solar cells have been over 20.0%. [14][15][16][17] Furthermore, perovskitebased photodetectors are being quickly developed as well. [18][19][20] The interface engineering using suitable interface materials is a powerful approach to improve the performance of perovskite photodetectors. [21][22][23][24][25] The graphene/perovskite hybrid photodetectors produced high performance with a responsivity up to 180 A W −1 , [23] and a monolayer graphene covered with a thin layer of dispersive perovskite islands resulted in an ultrahigh responsivity photodetector (≈6.0 × 10 5 A W −1 ). [26] However, the ratio of photocurrent and dark current (I light /I dark ) of these perovskite-based photodetector is very small, which is normally lower than 10. Very recently, it was reported that the CH 3 NH 3 PbI 3 /WS 2 heterostructure photodetectors could produce an I light /I dark of ≈10 5 and a responsivity of ≈17 A W −1 . [25] Organic semiconductor materials have the advantages of simple synthesis, low cost, large-scale, and low-temperature fabrication process, showing the great potentials for next-generation flexible electronic and photoelectronic devices. [27][28][29][30] Chen and co-workers demonstrated a photodetector based on CH 3 NH 3 PbI 3 and conjugated polymer (PDPP3T), of which the lifetime and stability were obviously improved owing to the protection of organic layer, while the performance parameters did not show obvious improvement, probably resulting from the low mobility of PDPP3T. [31] Dioctylbenzothieno [2,3-b] benzothiophene (C8BTBT) is an excellent organic semiconductor material with good air stability and ultrahigh hole carrier mobility. [32,33] Herein, we demonstrate that a CH 3 NH 3 PbI 3 / C8BTBT heterojunction produced by solution-processable method could be effectively used to fabricate high-performancePerovskite photodetectors are fabricated via structuring a perovskite/organic heterojunction with CH 3 NH 3 PbI 3 and a high-mobility and stable organic semiconductor dioctylbenzothieno [2,3-b] benzothiophene (C8BTBT), which possess broad range photoresponse from ultraviolet to near-infrared, fast response, and excellent stability. The CH 3 NH 3 PbI 3 /C8BTBT heterojunction photodetectors exhibit an excellent ratio of photocurrent to dark current, I light /I dark , as high as 2.4 × 10 4 , a high responsivity up to 24.8 AW −1 , and a fast response of about 4.0 ms. Meanwhile, the photodetectors can maintain 90% performance even exposed in ambient condition without encapsulation for 20 ...