To comparatively validate the functionality of quasi-2D HPs with designed compositions that NMF-based prediction and Gated-GPBO respectively suggested, we assess the performances of p-i-n type PVs employing these matrices as a photoactive layer; a device architecture of ITO / poly[bis(4-phenyl)(2,4,6trimethylphenyl)amine] (PTAA) / Poly(9,9-bis(3'-(N,N-dimethyl)-N-ethylammoiniumpropyl-2,7-fluorene)-alt-2,7-(9,9-dioctylfluorene))dibromide (PFN-Br) / quasi-2D HP / C60 / Bathocuproine (BCP) / Ag is used. Figure shows the current-voltage curves of the champion PVs employing the corresponding quasi-2D HP films. Without any optimizations, the quasi-2D HP film designed by Gated-GPBO demonstrates the highest PV performance with a PCE of 11.16%, showing ~15-60% enhancements compared to the performances of PV with NMF-predicted films (Detailed PV parameters are summarized in Table ). Such a higher PCE of the Gated-GPBOdesigned PV is majorly gained by the improvements in open-circuit voltage (VOC) and fill factor (FF). This indicates that the carrier loss is greatly suppressed in the Gated-GPBO-designed film, likely attributed to better chemical homogenization of the quasi-2D HP lattice. It should be noted that the films are synthesized at a low annealing temperature (95 o C), without any dedicated efforts in additional chemical and device engineering. This indicates that the Gated-GPBO-designed quasi-2D HP still has potential realizing high performances, on par with those of widely used large-bandgap sub-cells that are required for tandem applications . These results also validate the effectiveness of the Gated-GPBO for materials design used in this study, which can significantly accelerate the discovery of new functional materials realizing high PV performances from massive complex materials space.