The interface between the semiconductor and the dielectric layer plays a crucial role in organic field-effect transistors (OFETs) because it is at the interface that charge carriers are accumulated and transported. In this study, four zwitterionic benzoquinonemonoimine dyes featuring alkyl and aryl N-substituents were used to cover the dielectric layers in OFET structures. The best interlayer material, containing aliphatic side groups, increased charge carrier mobility in the measured systems. This improvement can be explained by the reduction in the number of the charge carrier trapping sites at the dielectric active layer interface from 1014 eV−1 cm−2 to 2 × 1013 eV−1 cm−2. The density of the traps was one order of magnitude lower compared to the unmodified transistors. This resulted in an increase in charge carrier mobility in the tested poly [2,5-(2-octyldodecyl)-3,6-diketopyrrolopyrrole-alt-5,5-(2,5-di(thien-2-yl)thieno [3,2-b]thiophene)] (DPPDTT)-based transistors to 5.4 × 10−1 cm2 V−1 s−1.