Atomic force microscopy was used to monitor the macroscopic deformation in a delaminated Ti3C2 paper electrode in situ, during charge/discharge in a variety of aqueous electrolytes to examine the effect of the cation intercalation on the electrochemical behavior and mechanical response. The results show a strong dependence of the electrode deformation on cation size and charge. The electrode undergoes a large contraction during Li+, Na+ or Mg2+ intercalation, differentiating the Ti3C2 paper from conventional electrodes where redox intercalation of ions (e.g. Li+) into the bulk phase (e.g. graphite, silicon) results in volumetric expansion. This feature may explain the excellent rate performance and cyclability reported for MXenes. We also demonstrated that the variation of the electromechanical contraction can be easily adjusted by electrolyte exchange, and shows interesting characteristics for the design of actuators based on 2D metal carbides.