LAUSR

Conjugated polymer design via random terpolymerization with irregular backbones has emerged as a strategy for stretchable organic electronics, requiring diverse molecular architectures to balance charge carrier mobility (μ) and stretchability. In this study, diketopyrrolopyrrole (DPP)‐based conjugated polymers with 0%, 5%, and 10% Pechmann dye (PDy) units, denoted as DP‐T0, DP‐T5, and DP‐T10, respectively, are introduced, and explore the impact of PDy on structural mobility and stretchability through experimental and computational analyses. Electrical measurements reveal hole mobilities ranging from 0.01 to 0.08 cm2 V⁻¹ s⁻¹, with a slight decrease as PDy content increases. Stretchability tests indicate significant improvements in DP‐T5 and DP‐T10 due to their loosely packed lamellar structures. Notably, DP‐T5 achieves a crack onset strain (εc) of 250% and a polarization dichroic ratio (PDR) of 2.4 under 200% strain, leading to a mobility ratio (μ200/μ0) exceeding 5. These results demonstrate that PDy incorporation enhances the mechanical stretchability of DPP‐based conjugated polymers while maintaining reasonable electronic performance. This work highlights the potential of PDy‐based random terpolymerization for developing stretchable polymer semiconductors.