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Highly flexible pseudocapacitors (PCs) have great potential in modern electronics such as portable and wearable devices. However, they are not yet mature enough to reach the market due to low energy density. In this study, for the first time, we are reporting an efficient synergetic approach by optimizing the feeding ratio of cobalt:gallium (Co:Ga) with a binder-free architecture composed by novel hexagonal-shaped nanoplates on carbon cloth (CC) substrate with high surface area to achieve high-energy electrode for asymmetric supercapacitor (ASC). Owing to the integrated strengths including enhanced electronic/ionic transportation and structural stability, the optimized sample with feeding ratio of Co:Ga = 1:2 (Co₁Ga₂O₄@CC) electrode exhibited excellent charge storage performance, including high capacitance of 1525 F g⁻¹ (915 C g⁻¹) at 5 A g⁻¹ with superb rate-capability and superior cycling stability of 95 …