Here, a simple active materials synthesis method is presented that boosts electrode performance and utilizes a facile screen‐printing technique to prepare scalable patterned flexible supercapacitors based on manganese hexacyanoferrate‐manganese oxide and electrochemically reduced graphene oxide electrode materials (MnHCF‐MnOx/ErGO). A very simple in situ self‐reaction method is developed to introduce MnOx pseudocapacitor material into the MnHCF system by using NH4F. This MnHCF‐MnOx electrode materials can deliver excellent capacitance of 467 F g−1 at a current density of 1 A g−1, which is a 2.4 times capacitance increase compared to MnHCF. In addition a printed, patterned, flexible MnHCF‐MnOx/ErGO supercapacitor is fabricated, showing a remarkable areal capacitance of 16.8 mF cm−2 and considerable energy and power density of 0.5 mWh cm−2 and 0.0023 mW cm−2, respectively. Furthermore, the printed patterned flexible supercapacitors also exhibit exceptional flexibility, and the capacitance remains stable, even while bending to various angles (60°, 90°, and 180°) and for 100 cycles. The flexible supercapacitor arrays integrated by multiple prepared single supercapacitors can power various LEDs even in the bent states. This approach offers promising opportunities for the development of printable energy storage materials and devices with high energy density, large scalability, and excellent flexibility.
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