Quasi-two-dimensional (q2D) conducting polymer thin film synergizes the advantageous features of long-range molecular ordering and high intrinsic conductivity, which are promising for flexible thin film-based micro-supercapacitors (MSCs). Herein, we present the high-performance flexible MSCs based on highly ordered quasi-two-dimensional polyaniline (q2D-PANI) thin film using surfactant monolayer assisted interfacial synthesis (SMAIS). Owing to high electrical conductivity, rich redox chemistry, and thin-film morphology, the q2D-PANI MSCs show high volumetric specific capacitance (ca. 360 F/cm³) and energy density (17.9 mWh/cm³), which outperform the state-of-art PANI thin-film based MSCs and promise for future flexible electronics.