Molecular doping, under certain circumstances, can be used to improve the charge transport in organic semiconductors through the introduction of excess charge carriers which can in turn negate unwanted trap states often present in organic semiconductors. Here, two Lewis basic indenopyrazine copolymers with large ionization potential (5.78 and 5.82 eV) are prepared to investigate the p-doping efficiency with the Lewis acid dopant, tris(pentafluorophenyl)borane, using organic thin-film transistors (OTFTs). The formation of Lewis acid–base complex between the polymer and dopant molecules is confirmed via optical spectroscopy and electrical field-effect measurements, with the latter revealing a dopant-concentration-dependent device performance. By adjusting the amount of p-dopant, the hole mobility can be increased up to 11-fold while the OTFTs’ threshold voltages are reduced. The work demonstrates an alternative doping mechanism other than the traditional charge transfer model, where the energy level matching principle can limit the option of dopants.