Organic−inorganic hybrid perovskites have attracted significant attention because of their distinguished optoelectronic properties, which can be applied in high-efficiency solar cells and light-emitting devices. A majority of the systematic studies on the regulation of the band gap in the family of organolead halide perovskites have focused on changing the compositions of halogens. However, mechanical compression provides a wider structural diversity without changing the composition. In this paper, fabrication of organic−inorganic hybrid perovskites (CH 3 NH 3 PbX 3 , X = Cl, Br, and I) is reported. The crystal structure, electronic properties, and optical band gap energies of the synthesized perovskites were investigated. Also, the effects of changing the external pressure on the band gap of CH 3 NH 3 PbX 3 , X = Cl, Br, and I were studied. The results indicate an important progress in tuning the band structure and optoelectronic properties of organometal halide perovskites via pressure engineering, which brings forward substantial implications for practical device applications. Investigation of the optical band transition induced through pressure could provide a different perspective on studying the perovskite materials.