Broadband photodetectors possess enormous potentials for diverse applications while it is generally subjected to a lack of active materials with high performances under user-friendly conditions. Bismuth-based perovskites are promising and demonstrate better air stability than lead halide perovskites against moisture, heat, and light. In the present work, lead-free all-inorganic hexagonal Cs 3 Bi 2 I 9 perovskite nanocrystals are successfully fabricated via a modulated colloidal synthetic route. The Cs 3 Bi 2 I 9 nanocrystals are monodispersed with a size of ≈28 nm, which are applied for the construction of flexible Cs 3 Bi 2 I 9 detector and vertical heterogeneous structured photo detector of p-Si/Cs 3 Bi 2 I 9 /graphene. The flexible detector not only demonstrates excellent detective performance, but also yields high-resolution photographs as an imaging sensor. The p-Si/Cs 3 Bi 2 I 9 /graphene photodetector exhibits broad spectral response from ultraviolet to infrared light (254−1064 nm) with microsecond response time (31/34 µs). In particular, it performs with a high responsivity of 23.6 A W −1 and a high specific detectivity of 1.75 × 10 13 Jones under 650 nm illumination even in weak light intensity as low as 1 µW cm −2 , and exhibits excellent stability in ambient air, which is obviously ahead of the previously reported work. In addition, finite element analysis further demonstrates the excellent optoelectronic properties of Cs 3 Bi 2 I 9 materials and the broad spectral response of vertical heterojunctions.