Highly regioregular (RR) poly(3-hexylthiophene)s PHTs are known to exhibit excellent electrical properties in comparison to chemically identical but regiorandom (rr) PHTs. In this study, distinct RR (97% and 55%)-graded PHTs are subjected to solution blending to spontaneously separate the high-RR PHT chains from the low-RR PHT media and develop highly conjugated nanodomains in both solution and film. In the spun-cast blend films, the rr PHT matrix imparts sufficient deformability of the channel layer required for stretchable organic thin-film transistors (OTFTs), compared to neat RR PHTs and blends with a deformable polymer. OTFTs including RR PHT/rr PHT blend films show excellent hole mobility (µ) values up to 0.13 cm 2 V −1 s −1 , surpassing that of the best RR PHT films (0.026 cm 2 V −1 s −1 ) fabricated by ultrasound solution pretreatment. Furthermore, a 50% stretched RR PHT/rr PHT film maintains ≈55% of its µ value at no strain, while RR PHT films show a sudden decrease in µ even at 10% stretch. The simple blending approach imparts deformability to π-conjugated polymer films for application in stretchable OTFTs.