Transition metal oxides (TMOs) are widely used in the development of high-energy-density devices due to their multiple oxidation states and their frequent heterostructuring with carbon-based materials. However, the synthesis process often leads to severe nanoparticle agglomeration and weak synergistic effects with carbon-based templates, thereby limiting their application potential. In this study, we constructed graphitic carbon nitride (GCN) nanosheets/ZnO nanoflowers (NFs) structures with high TMOs loading by utilizing GCN nanosheets, which are rich in surface nitrogen content, as enriched templates for metal ions in conjunction with ultrasonic cavitation. Compared with GCN nanosheets/ZnO nanoparticles (NPs), the ZnO NFs exhibited vertical growth and a fluffy structure on a 2D material template, which resulted in high electronic conductivity, a large effective surface area, hierarchical pores, and strong synergistic interactions with GCNs, thus improving electrochemical performance. This structural enhancement enabled the GCN/ZnO NFs electrodes to achieve a high specific capacitance of 1524F g−1 at a current density of 1 A g−1 in a three-electrode supercapacitor system. Additionally, we formulated GCN/ZnO NFs into electronic inks and used them for the mass production of flexible supercapacitors with the aid of dispensing printing technology. These flexible supercapacitors retained 94% of their specific capacitance even under extreme conditions of 90° torsion. Our proposed strategy of modulating TMOs and 2D structures can create active electrode materials with higher loading capacities, thereby enabling comprehensive customization in material design and device preparation processes.
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