LAUSR

Intrinsically stretchable polymer semiconductors are highly demanding for flexible electronics. However, it still remains challenging to achieve synergy between intrinsic stretchability and charge transport property properly for polymer semiconductors. In this paper, terpolymers are reported as intrinsically stretchable polymeric semiconductors with good ductility and high charge mobility simultaneously by incorporation of non‐centrosymmetric spiro[cycloalkane‐1,9′‐fluorene] (spiro‐fluorene) units into the backbone of diketopyrrolopyrrole (DPP) based conjugated polymers. The results reveal that these terpolymers show obviously high crack onset strains and their tensile moduli are remarkably reduced, by comparing with the parent DPP‐based conjugated polymer without spiro‐fluorene units. They exhibit simultaneously high charge mobilities (>1.0 cm2 V−1 s−1) at 100% strain and even after repeated stretching and releasing cycles for 500 times under 50% strain. The terpolymer P2, in which cyclopropane is linked to the spiro‐fluorene unit, is among the best reported intrinsically stretchable polymer semiconductors with record mobility up to 3.1 cm2 V−1 s−1 at even 150% strain and 1.4 cm2 V−1 s−1 after repeated stretching and releasing cycles for 1000 times.