As an environmentally friendly metal-halide double perovskite, Cs 2 AgBiBr 6 has been gaining emerging interest to replace the traditional lead perovskite in photovoltaics. However, the drawback of indirect large energy gap has limited Cs 2 AgBiBr 6 from being applied in efficient solar cell devices. Compositionally tuning halide is one of the most convenient methods to narrow down its energy gap, within which iodine is the most ideal candidate as a dopant. However, not much experimental research has been reported so far on iodine-doped Cs 2 AgBiBr 6 due to phase segregation. Herein, we first use Raman spectroscopy as the technique to systematically discover the structural dynamic properties in Cs 2 AgBi(Br 1−x I x ) 6 (x ≤ 0.15) and to understand the mechanism for their phase segregation. We investigate both the compositional effects through doping and the illumination effects through tuning Raman laser's intensities or excitation energies, where we reveal that the leading factor for phase segregation is likely due to the changes in intrinsic lattice strain. Structural analysis demonstrates that the compositional transition point is at x = 0.07, signaling with the rise of new phonon modes. The strain-based hidden mechanisms have been discussed from an atomic level and micro/nanoscale. We also propose a few guidelines to engineer the strain and to optimize the advantages of such lead-free perovskites for future applications.