of pseudocapacitance storage. According to previous studies, LDH is an inorganic anion conductor with a charged brucite-like metal hydroxide layer structure, which is composed of divalent (M 2+) and trivalent (M 3+) metal ioncentered octahedrons. In the accessible interlayer channel, replacing M 2+ with M 3+ can results in the insertion of positively charged and negatively charged counterions (A n−), and some anions and uncharged molecules are in the interlayer, which play a crucial role in ion conduction. [18-22] In particular, the combination of the anion exchange performance and 2D structure improves the electron/ ion transmission efficiency and kinetics during charge-discharge process. Therefore, while maintaining the 2D layered structure, LDHs can also adjust the transition metal charge, which can increase the pseudocapacitance of the electrode material. [23-29] Moreover, NiAl-LDHs have attracted considerable attention because of their higher theoretical specific capacitance, lower cost, easy to be synthesized and promising materials for advanced electrodes. Some studies had shown that Ni/Al ratio has a significant influence on its structure, morphology, ion transport mechanics, interlayer phenomena and performance, and the specific capacitance and charge-discharge cycling performances can be further increased by controlling the ratio of Al/Ni. [2] However, the interface contacts and poor electrical conductivity widely affects electron transport and ion migration. Although the NiAl-LDHs electrode material has high reactivity and high theoretical capacitance, its insulation and large interface contact area lead to high impedance, which affects the pseudocapacitance storage performance. [30] To solve the above issues, one of the strategies used to improve the conductivity of LDHs is the introduction of a conductor with cross-link nanoscale active ingredients (such as graphene or carbon nanotubes). [31-35] The MAX phase is a ternary ceramic material, where M, A, and X represent transition metal elements, elements of the third or fourth main group, and C or N, respectively. MXene is obtained by etching the MAX phase with HF. As a new potential 2D material, with the 2D structure, the electrical conductivity of metal and the hydrophilic surface, MXene shows excellent performance in the fields of Multifarious layered electrode materials are attracting increased attention in the field of energy storage because of their high specific surface and interlayer modifiability. However, the natural tendency to be re-superimposed and the inherent disadvantages of a single layered electrode significantly affect electronic transport and ion migration. Considering the poor electrochemical performance and low structural stability, a novel MXene@PDDA/NiAl-LDHs hybrids as supercapacitor electrode via an electrostatic-assembled approach is elaborately designed. The alternate MXene and PDDA/NiAl-LDHs layers with 3D interconnected networks architectures could ensure intimate contact to efficiently take advantage of high electron cond...