The power conversion efficiency of the perovskite-based solar cells has been rapidly exceeding 23% in the past few years. In the paper, the electronic and optical properties of the doped series MAPb1−αXαI3−βYβ (X = Ge, Sn; Y = Cl, Br) are explored for ascendant absorption capability. Hybrid density functional has been conducted to obtain exact electronic property. The defect formation energy, with the maximal value of −2.221 eV, indicates that all the doped series can be readily synthesized. Moreover, the charge density distributions suggest that photogenerated holes are easily transferred to the adjacent hole transport layer in Cl/Br-mono than in the others. Furthermore, it is clearly revealed that absorption coefficients of perovskite-based compounds, including the Ge-mono, Sn-mono, Ge–Cl, and Ge–Br, are significantly enhanced in the whole visible-light range and even near infrared. Our simulations pave a new way to deepen the understanding of the intrinsic characteristics of perovskite materials, and d...