A new tandem architecture for printable photovoltaics using a versatile organic nanocomposite containing photoactive and interfacial materials is demonstrated. The nanocomposite forms an ideal self-organized recombination layer via a spontaneous vertical phase separation, which yields a simplified tandem structure fabricated with only four component layers and a high tandem efficiency of 10.8%.

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Because the fabrication process of organic tandem solar cells described by K. Lee and co‐workers on page 1408 is similar to the process for the cooking of cakes, the manufacturing process of cakes (i.e., tandem polymer solar cells) fabricated from various color doughs (i.e., organic electronic inks) is illustrated in the back‐cover design so that the concept can be easily understood. To keep the scientific concept that simplifies tandem structures, the focus is on “spontaneous vertical phase separation of mixed doughs” (i.e., a mixture of organic electronic inks), which is the essence of the process.