摘要
Simultaneously achieving high sensitivity and ultrafast response is a challenge for photodetectors, a bottleneck further compounded by the environmental toxicity of lead‐based halide perovskite photodetectors. Herein, we overcome these limitations via a lead‐free, quasi‐2D germanium‐based halide perovskite, PEA 2 MA 3 Ge 4 I 13 . Distinguished by its non‐centrosymmetric structure, this material exhibits robust ferroelectricity, pyroelectricity, and second‐order nonlinear optical susceptibility. By coupling the pyroelectric effect and photovoltaic effect, we successfully decouple the conventional sensitivity‐speed trade‐off, achieving a very high specific detectivity of 6.3 × 10 14 Jones alongside a remarkable response time in ns scale. The practical viability of these devices is demonstrated through advanced applications in tens of centimeter‐level (1 ns light travelling time) light detection and ranging (LiDAR) and fast visible light communication (VLC). This work establishes a compelling strategy for realizing next‐generation, environmentally benign, and high‐performance optoelectronics.