• • Temperature-controlled crystallization of TQDPT single crystals yields a morphological transition from needle-like to plate-like structures, with average widths tunable from 2.8 μm to 30.1 μm across 15–35°C, enabling deterministic dimensional control for OFET fabrication.
• • Plate-like crystals grown at 25°C exhibit an order-of-magnitude enhancement in carrier mobility compared to needle-like counterparts, directly linking growth temperature to electronic performance.
• • Crystals grown at 35°C produce broader plate-like crystals with improved carrier mobility and device stability, indicating that higher temperatures within the studied range optimize both charge transport and operational robustness.
• • The study establishes a predictive framework linking growth temperature to morphological evolution and device performance, addressing the lack of quantitative guidelines for template-free crystallization of organic semiconductors.