© 2020 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim Oriented microstructures are widely found in various biological systems for multiple functions. Such anisotropic structures provide low tortuosity and sufficient surface area, desirable for the design of high-performance energy storage devices. Despite significant efforts to develop supercapacitors with aligned morphology, challenges remain due to the predefined pore sizes, limited mechanical flexibility, and low mass loading. Herein, a wood-inspired flexible all-solid-state hydrogel supercapacitor is demonstrated by morphologically tuning the aligned hydrogel matrix toward high electrode-materials loading and high areal capacitance. The highly aligned matrix exhibits broad morphological tunability (47–12 µm), mechanical flexibility (0°–180° bending), and uniform polypyrrole loading up to 7 mm thick matrix. After being assembled into a solid-state supercapacitor, the areal capacitance reaches 831 mF cm−2 for the 12 µm matrix, which is 259% times of the 47 µm matrix and 403% times of nonaligned matrix. The supercapacitor also exhibits a high energy density of 73.8 µWh cm−2, power density of 4960 µW cm−2, capacitance retention of 86.5% after 1000 cycles, and bending stability of 95% after 5000 cycles. The principle to structurally design the oriented matrices for high electrode material loading opens up the possibility for advanced energy storage applications.