Abstract: Two-dimensional Ti₃C₂T_x exhibits outstanding rate property and cycle performance in lithium-ion capacitors (LICs) due to its unique layered structure, excellent electronic conductivity, and high specific surface area. However, like graphene, Ti₃C₂T_x restacks during electrochemical cycling due to hydrogen bonding or van der Waals forces, leading to a decrease in the specific surface area and an increase in the diffusion distance of electrolyte ions between the interlayer of the material. Here, a transition metal selenide MoSe₂ with a special three-stacked atomic layered structure, derived from metal–organic framework (MOF), is introduced into the Ti₃C₂T_x structure through a solvothermal method. The synergic effects of rapid Li⁺ diffusion and pillaring effect from the MoSe₂ and excellent conductivity from the Ti₃C₂T_x sheets endow the material with excellent electrochemical reaction kinetics and capacity. The composite Ti₃C₂T_x@MoSe₂ material exhibits a high capacity over 300 mAh·g⁻¹ at 150 mA·g⁻¹ and excellent rate property with a specific capacity of 150 mAh·g⁻¹ at 1500 mA·g⁻¹. Additionally, the material shows a superior capacitive contribution of 86.0% at 2.0 mV·s⁻¹ due to the fast electrochemical reactions. A Ti₃C₂T_x@MoSe₂//AC LIC device is also fabricated and exhibits stable cycle performance.