This study presents a detailed investigation into optimizing the novel perovskite Mg3AsBr3 through uniaxial stress for enhanced performance in solar and optoelectronic applications. Using Density Functional Theory (DFT), we examined its structural, electronic, and optical properties under uniaxial stress from 0.5 to 5.0 GPa. Key findings include the tuning of the material’s bandgap from 1.485 eV (without stress) to an optimized range closer to 1.13581 eV under 5.0 GPa, demonstrating potential for improved solar cell efficiency. Our findings reveal a nuanced response of the material’s absorption coefficients at critical energies of 2.92 eV and 4.0 eV, where a descending trend with increasing pressure was observed, indicating a plateau at 1.5 GPa and an anomalous increase at 2.5 GPa. This behavior underscores the significance of stress between 2.5 GPa to 5.0 GPa in tailoring the optical responses essential for enhancing solar absorption efficiency in the ultraviolet to visible light range (300–800 nm). Notably, the dielectric constant increased gradually with stress, peaking at 6.003 under 0.5 GPa and slightly diminishing at 5.0 GPa, suggesting enhanced polarization and intrinsic response to electric fields under mechanical stress. Our research highlights the potential of stress engineering in optimizing perovskite materials for renewable energy applications, offering a pathway to high-efficiency, low-cost solar cells.