As a conductive polymer, polyaniline (PANI) has been broadly utilized as an electrode material for highperformance SCs thanks to its large specific capacitance, [3,4] outstanding flexibility, [5][6][7] and environmental stability, let alone its easy synthesis. [8][9][10] Although PANI exhibits a satisfying performance in SCs, its relatively low electric and ionic conductivity resulting from agglomeration will lead to a sluggish redox reaction and thus a deteriorated capacitance under high current density. [11][12][13] This problem should weaken the practicality of PANI electrodes to a certain degree. According to the successful experience of other electrodes that have solved the similar problems, [14][15][16] it is preferable to combine the pseudocapacitive PANI with some conductive and porous materials, which can assist PANI to achieve its full potential via the synergistic effects. [10,[17][18][19] For instance, 2D materials (e.g., graphene) with large and adjustable surfaces could load a large number of PANI nanoparticles with good homogeneity via different means, guaranteeing a fast redox reaction and then a decent rate capability. [17,18,[20][21][22] As an important member of 2D materials, antimonene (Sb) nanosheets present not only a large surface area and high conductivity, [23,24] but also excellent mechanical strength and flexibility. [25,26] A preliminary researchIn virtue of the high electrochemical activity and inherent flexibility, polyaniline (PANI) is an ideal electrode material for flexible supercapacitors (SCs). However, in practical applications, the inevitable agglomeration of PANI leads to low capacitance, poor rate performance, and cycling stability. Here, antimonene (Sb) nanosheets with ultrathin thickness, excellent mechanical strength, and flexibility are introduced into the carbon nanotube (CNT) framework for PANI electrodeposition via simple vacuum filtration, which enables the continuous and uniform growth of PANI. The resultant free-standing Sb/CNT/PANI electrode can thus exhibit a high specific capacitance of 578.57 F g −1 together with a high rate capability. Besides, thanks to the introduction of Sb nanosheets, the agglomeration of PANI during the electrodeposition is improved, which correspondingly alleviates the structural deterioration of PANI during repeated charge/discharge. Thus, the flexible SC assembled by Sb/CNT/PANI electrodes demonstrates both an impressive specific capacitance of 416 F g −1 and outstanding cycling stability over 12 000 cycles. Moreover, this SC device can have a practical self-healing function by employing self-healable polyurethane. The facile strategy reported herein sheds light on the design of high-performance flexible SCs, catering to the needs of portable and wearable electronics.