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The data included in this article is based on additional supporting information presented in our recent publication Komilian et al. [1]. The role of acceptor material (PC71BM) in restructuring copolymer PBDTTT-EFT from its relaxed pristine structure to interfaces suitable for exciton dissociation is discussed. The analysis of data indicates that the impact of acceptor material on nanostructuring initiates concurrent processes some of which supports and some impedes charge extractions. Therefore, this manuscript is designed to identify these processes and give and account of their impact on power conversion efficiency.

The realization of solution processed polymer/fullerene as a constituent material for an active layer of solar cell raises a fundamental question relating to the nanostructure formation of these devices and its impact on a device's electrical parameters. To have an insight in nanomorphology and nanostructuring, Raman mapping of the scanned surface after each successive chemical etching is performed to build a picture of a vertical profile. To further support this technique, grazing incidence X‐ray diffraction (GIXRD) analysis on an etched surface is also performed. The data generated reveals an accurate correlation between these two techniques. To complete these investigations the impact of blend composition ratios on a nanostructure reveals that fullerene plays a critical role in self‐organization facilitating the rotation of a favorable face‐on the orientation to edge‐on allowing the migration of PC71BM towards the film surface. The impact of these investigations on electrical parameters has been addressed.