The commercialized light-sensitive materials for PDs, such as silicon and InGaAs, are however produced by energy-consuming high-temperature methods. [6][7][8] Solutionpossessed metal halide perovskites have been exploited as low-cost alternatives that are able to present surpassing sensitivity and linear dynamic range in broad spectral regions, including the ultraviolet, visible (vis), and near-infrared (NIR). [9,10] The archetypal methylammonium lead iodide (MAPbI 3 ) perovskite has shown high sensitivity and low noise for visible light detection, but suffered from blindness in the NIR region due to the cutoff wavelength of ≈800 nm. [11,12] As an alternative, tin-lead alloyed perovskites experiencing spectral response of over 1000 nm, are particularly suitable for broadband photodetection with good electrical property and environmental stability. [13] Taking MASn x Pb 1-x I 3 as an example, the resulting optical bandgap (E g ) can be finely tuned between 1.17 ≈ 1.55 eV by changing the Sn content in the composition. [14][15][16] Nevertheless, the performance of tin-lead perovskite photodetectors (PPDs) is mostly inferior compared with the lead-based counterparts, and their versatility is normally relied on several crucial factors, including the response time, sensitivity to low brightness, detection band, and reliability, which is hard to be achieved simultaneously. [17][18][19][20][21] The strain that relates to the deformation of materials is ubiquitously existed in thin-film perovskite devices. Residual strain is usually caused by the unequal thermal expansion coefficients at the perovskite/substrate interface and could be reduced by modifying the substrates or annealing procedure. [22,23] Recent studies revealed the opposite impact of in-plane tensile and compressive strains, while the latter one was found to be beneficial for the stabilization and charge transport of hybrid perovskites. [24] Also, there is a microstrain in bulk perovskite, i.e., lattice strain, which is a measure of the lattice constant distribution arising from microscopic crystal imperfections, such as vacancy and dislocation. [25][26][27] Local lattice mismatch of perovskites would generate a large microstrain, which distorts the crystal structure by tilting, expansion, or shrinkage of the octahedral network, and even lead to phase Tin-lead alloyed perovskites with broadband absorption over 1000 nm, are suitable for UV-vis-NIR light detection that rivals the crystalline silicon semiconductors. These alloyed perovskites usually experience local lattice distortion and inherent lattice strain, which affect the electronic band structures and introduce detrimental trap states subsequently. To date, the lattice strain and its impact on the physical properties of tin-lead alloyed perovskites are still less understood. Herein, it is shown that the lattice strain contributes substantially to the band edge electronic structure of multication tin-lead alloyed perovskites by tilting the metal halide octahedral configuration. It has been found that th...