The first set of GAs designed new small-molecule NFAs. 1,244 NFAs were discovered with a predicted PCE greater than 18%, with the highest PCE predicted to be 20.8%. NFAs with a fusedring backbone structure and π-conjugated spacers tended to yield higher efficiencies. Interesting motifs appeared frequently in high-performing NFAs, such as diphenylamine side chains on the core that can lead to strong broad absorption, and 3D terminal groups, which is thought to lead to efficient charge transport pathways due to good crystal packing. Another GA was used to find donor polymers complementary to the top NFAs discovered thus far. The top candidates revealed tailored sequences can lead to higher performance than the prevailing alternating copolymer strategy.