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Heteroatom doping is considered an effective method to substantially improve the electrochemical performance of Ti₃C₂T_x MXene for supercapacitors. Herein, a facile and controllable strategy, which combines heat treatment with phosphorous (P) doping by using sodium phosphinate (NaH₂PO₂) as a phosphorus source, is used to modify Ti₃C₂T_x. The intercalated ions from NaH₂PO₂ act as “pillars” to expand the interlayer space of MXene, which is conducive to electrolyte ion diffusion. On the other hand, P doping tailors the surface electronic state of MXene, optimizing electronic conductivity and reducing the free energy of H⁺ diffusion on the MXene surface. Meanwhile, P sites with lower electronegativity owning good electron donor characteristics are easy to share electrons with H⁺, which is beneficial to charge storage. Moreover, the adopted heat treatment replaces –F terminations with O-containing groups, which enhances the hydrophilicity and provides sufficient active sites. The change in surface functional groups increases the content of high valence-stated Ti with a high electrochemical activity that can accommodate more electrons during discharge. Synergistic modification of interlayer structure and chemical state improves the possibility of Ti₃C₂T_x for accommodating more H⁺ ions. Consequently, the modified electrode delivers a specific capacitance of 510 F g⁻¹ at 2 mV s⁻¹, and a capacitance retention of 90.2% at 20 A g⁻¹ after 10,000 cycles. The work provides a coordinated strategy for the rational design of high-capacitance Ti₃C₂T_x MXene electrodes.