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The incorporation of insulating polymers into conjugated polymers has been widely explored as a strategy to improve mechanical properties of flexible organic electronics. However, phase separation due to the immiscibility of these polymers has limited their effectiveness. In this study, we report the discovery of multiple non‐covalent interactions that enhances the miscibility between insulating and conjugated polymers, resulting in improved mechanical properties. Specifically, we have added polyvinyl chloride (PVC) into the conjugated polymer PM6 and observed a significant increase in solution viscosity, indicative of favorable miscibility between these two polymers. This phenomenon has been rarely observed in other insulating/conjugated polymer composites. Thin films of PM6/PVC exhibit a much‐improved crack‐onset strain of 19.35 %, compared to 10.12 % for pristine PM6 films. Analysis reveal that a "cyclohexyl‐like" structure formed through dipole‐dipole interactions and hydrogen bonding between PVC and PM6 acted as a cross‐linking site in the thin films, leading to improved mechanical properties. Moreover, PM6/PVC blend films have demonstrated excellent thermal and bending stability when applied as an electron donor in organic solar cells. These findings provide new insights into non‐covalent interactions that can be utilized to enhance the properties of conjugated polymers and may have potential applications in flexible organic electronics. [ABSTRACT FROM AUTHOR]

Two kinds of small molecular dyads (SMDs) based on trithiophene-benzodithiophene-rhodanine (DR3TBDT) main backbone and PBI termini, named SMD2-C6 and SMD2-C12, were designed with different lengths of alkyl linkers (C 6 H 12 and C 12 H 24). The length effect of alkyl linkers on the photovoltaic performance of the two SMDs have been systematically studied. The results show that the length of alkyl linkers can simutaneously tune the energy levels and phase separation in molecular dyad thin films. As a result, a power conversion efficiency of 1.33% was obtained for SMD2-C12 based single-component organic solar cells (SCOSCs), showing higher open-circuit voltage, short-circuit current density, and fill factor than those of SMD2-C6 based devices. Our findings provide a strategy for designing new SMDs and reveal the importance of alkyl linkers' length on the morphology of SMDs toward improved SCOSC performance. Small molecular dyads based on DR3TBDT backbone and PBI end groups with varying alkyl linker lengths have been developed for application in single-component organic solar cells. [Display omitted] • Two molecular dyads based on a donor backbone and perylene bisimides end groups were developed. • Different alkyl linkers as C 6 H 12 and C 12 H 24 were introduced. • Longer alkyl linkers were found to improve the nanophase separation and provided higher efficiency in single-component organic solar cells. [ABSTRACT FROM AUTHOR]