The printing of large‐area organic solar cells (OSCs) has become a frontier for organic electronics and is also regarded as a critical step in their industrial applications. With the rapid progress in the field of OSCs, the highest power conversion efficiency (PCE) for small‐area devices is approaching 15%, whereas the PCE for large‐area devices has also surpassed 10% in a single cell with an area of ≈1 cm2. Here, the progress of this fast developing area is reviewed, mainly focusing on: 1) material requirements (materials that are able to form efficient thick active layer films for large‐area printing); 2) modular designs (effective designs that can suppress electrical, geometric, optical, and additional losses, leading to a reduction in the PCE of the devices, as a consequence of substrate area expansion); and 3) printing methods (various scalable fabrication techniques that are employed for large‐area fabrication, including knife coating, slot‐die coating, screen printing, inkjet printing, gravure printing, flexographic printing, pad printing, and brush coating). By combining thick‐film material systems with efficient modular designs exhibiting low‐efficiency losses and employing the right printing methods, the fabrication of large‐area OSCs will be successfully realized in the near future.

The high efficiency all-small-molecule organic solar cells (OSCs) normally require optimized morphology in their bulk heterojunction active layers. Herein, a small-molecule donor is designed and synthesized, and single-crystal structural analyses reveal its explicit molecular planarity and compact intermolecular packing. A promising narrow bandgap small-molecule with absorption edge of more than 930 nm along with our home-designed small molecule is selected as electron acceptors. To the best of our knowledge, the binary all-small-molecule OSCs achieve the highest efficiency of 14.34% by optimizing their hierarchical morphologies, in which the donor or acceptor rich domains with size up to ca. 70 nm, and the donor crystals of tens of nanometers, together with the donor-acceptor blending, are proved coexisting in the hierarchical large domain. All-small-molecule photovoltaic system shows its promising for high performance OSCs, and our study is likely to lead to insights in relations between bulk heterojunction structure and photovoltaic performance.

Minimizing energy loss is of critical importance in the pursuit of attaining high-performance organic solar cells. Interestingly, reorganization energy plays a crucial role in photoelectric conversion processes. However, the understanding of the relationship between reorganization energy and energy losses has rarely been studied. Here, two acceptors, Qx-1 and Qx-2, were developed. The reorganization energies of these two acceptors during photoelectric conversion processes are substantially smaller than the conventional Y6 acceptor, which is beneficial for improving the exciton lifetime and diffusion length, promoting charge transport, and reducing the energy loss originating from exciton dissociation and non-radiative recombination. So, a high efficiency of 18.2% with high open circuit voltage above 0.93 V in the PM6:Qx-2 blend, accompanies a significantly reduced energy loss of 0.48 eV. This work underlines the importance of the reorganization energy in achieving small energy losses and paves a way to obtain high-performance organic solar cells.

Slot‐die coating is generally regarded as the most effective large‐scale methodology for the fabrication of organic solar cells (OSCs). However, the corresponding device performance significantly lags behind spin‐coated devices. Herein, the active layer morphology, flexible substrate properties, and the processing temperature are optimized synergistically to obtain high power conversion efficiency (PCE) for both the flexible single cells and the modules. As a result, the 1 cm2 flexible devices produce an excellent PCE of 12.16% as compared to 12.37% for the spin‐coated small‐area (0.04 cm2) rigid devices. Likewise, for modules with an area of 25 cm2, an extraordinary PCE of 10.09% is observed. Hence, efficiency losses associated with the upscaling are significantly reduced by the synergistic optimization. Moreover, after 1000 bending cycles at a bending radius of 10 mm, the flexible devices still produce over 99% of their initial PCE, whereas after being stored for over 6000 h in a glove box, the PCE reaches 103% of its initial value, indicating excellent device flexibility as well as superior shelf stability. These results, thus, are a promising confirmation the great potential for upscaling of large‐area OSCs in the near future.

For the preparation of flexible organic solar cells (OSCs), the Roll‐to‐Roll slot‐die coating technique is preferable. Herein, a sequential slot‐die (SSD) coating strategy to fabricate flexible OSCs using non halogenated solvent under ambient atmosphere, is developed. The coating order of the active layer materials shows great influence on the performance of OSCs. It is found that, compared with the one‐step coating, the power conversion efficiency (PCE) of devices with an area of 0.75 cm2, and fabricated by SSD coating process with the polymer as the first layer, is enhanced from 4.86 to 5.51% for the binary system, whereas from 6.09 to 7.32% for the ternary system, showing an increase of 13 and 20% in PCE, respectively. For the devices with a standard small area of 4 mm2 and large area of 1 cm2, PCE as high as 9.36 and 7.11% are obtained, respectively, which are among the top value for flexible devices fabricated by slot‐die coating. It turns out that the SSD coating process with the polymer as the first layer assists pre‐aggregation of the polymer to form better crystal domains with face‐on orientation. Therefore, a sequential deposition strategy could provide a new means for manufacturing the high efficiency flexible OSCs.

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As described by Zhixiang Wei and co‐workers in article number 1805089, for large‐area organic solar cells, high active‐layer thickness tolerability is generally required, the methods to reduce power conversion efficiency losses are critical, and printing methods suitable for roll‐to‐roll printing are highly important. By combining material requirements, modular designs, and printing methods, the application of organic solar cells will be successfully realized in the near future.

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