Interface modification with a particular triptycene molecule that spontaneously forms a highly uniform molecule layer is a promising technique for realizing high-performance flexible organic thin-film transistors (OTFTs). Previous studies have shown that the triptycene-modified polymer surface enhances the crystallinity of the small-molecule organic semiconductor (OSC), DNTT (dinaphtho[2,3-b:2′,3′-f]thieno[3,2-b]thiophene), resulting in improved mobility. However, to date, the effectiveness of triptycene modification for the other OSCs has not been confirmed. Here, we report on the positive effect of triptycene layers on four different thienoacene-based OSCs (C10-DNTT, DPh-DNTT, C8-BTBT ([1]benzothieno[3,2-b][1]benzothiophene), and DPh-BTBT) in OTFTs. Regardless of the OSC type, triptycene-modified OTFTs are found to improve the field-effect mobility. A maximum effective mobility enhancement of 20-fold was obtained for C10-DNTT OTFTs. Furthermore, detailed observations of the surface morphology of the OSCs via scanning electron microscopy revealed that the crystal grain size of the OSC thin films can be increased when triptycene modification is conducted.