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Ion pre-intercalation regulating the tunnel structure of electrode materials accelerates Zn2+ insertion kinetics to realize a high energy storage contribution of Zn-ion batteries. However, electrostatic interaction induced by the pre-intercalated cation and multivalent Zn2+ ions hinders the insertion of Zn2+/H+. In order to retain the negative interlayer surface, herein, OTf− anions were intercalated into the confined spacing by MXene via an electrochemical-driven method. Without changing the potential state of the interlayer spacings, OTf− anion induced a regulated interlayer distance, and a higher oxidation state of V based on the space occupation and the electron transfer mechanism. Consequently, the zinc ion storage capacity of V 2 CT x MXene increases from 125.2 to 288.7 mAh/g at 0.5 A/g. Interestingly, the negatively charged MXene surface was still intact, which presents lower diffusion barriers of the Zn2+ ions. The merits of anion pre-intercalation are highlighted and provide new insights into the ion storage function-oriented design of MXene. V 2 CT x MXene electrodes with high performance of zinc ion transport and storage ability were constructed by pre-intercalated OTf− via a potential-controlled method. [Display omitted] • Electrostatic interaction was utilized to realize anion intercalated V 2 CT x MXene. • Anion intercalation modulation relationship was investigated based on Zn ion storage behavior. • These pre-intercalated anions control the charge distribution of MXene's interlayer and improve the electrode function. [ABSTRACT FROM AUTHOR]