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General design principles of donor–acceptor block copolymers are reviewed and specific results arising from block copolymers consisting of semicrystalline poly(3-hexylthiophene-2,5-diyl) (P3HT) blocks of appreciably high molecular weight and acceptor blocks carrying pendant perylene bisimides or fullerene derivatives are summarized. The chapter is structured according to the building blocks P3HT, poly(perylene bisimide acrylate), and a polystyrene copolymer grafted with phenyl-C61-butyric acid methyl ester used for the synthesis of the corresponding block copolymers, and in each part the synthetic challenges, structure formation, and consequences for charge transport, and in some cases photovoltaic properties, are addressed. [ABSTRACT FROM AUTHOR]