Abstract 1D metal halide perovskites (MHPs) are known as excellent candidates for fabricating high‐performance optoelectronic devices, ranging from lasers to photodetectors (PDs). Nevertheless, their inherent limitations, such as high binding energy and limited carrier mobility, have restricted their further improvement in performance. To tackle this issue, hybrid MHP microwires (MWs) are fabricated by combining MHP MWs and an organic semiconductor via a facile self‐assembly method, forming a radial heterojunction. Meanwhile, an ultrathin insulating organic layer is introduced as an interlayer between MHP MWs and the organic semiconductor. The synthesized hybrid MWs are further applied in rigid and flexible PDs, which demonstrated a high light/dark current on‐off ratio (>2 × 10 5 ), a high responsivity (>400 A W −1 ), and robust bending stability. These impressive results make the hybrid MHP MWs with the unique radial heterostructure promising building blocks for high‐performance future optoelectronics.