Atomic force microscopy was used to monitor the macroscopic deformation in a delaminated Ti 3 C 2 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 Mg 2 + intercalation, differentiating the Ti 3 C 2 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 1 3 5 7 (J. Come), blackjm@ornl.gov (J.M. Black), mrl69@drexel.edu (M.R. Lukatskaya), naguibma@ornl.gov (M. Naguib), mbeidaghi@coe.drexel.edu (M. Beidaghi), rondinoneaj@ornl.gov (A.J. Rondinone), sergei2@ornl.gov (S.V. Kalinin), wesolowskid@ornl.gov (D.J. Wesolowski), gogotsi@drexel.edu (Y. Gogotsi), balken@ornl.gov (N. Balke).Nano Energy (]]]]) ], ]]]-]]] Please cite this article as: J. Come, et al., Controlling the actuation properties of MXene paper electrodes upon cation intercalation, Nano Energy (2015), http://dx.doi.org/10.1016/j.nanoen.2015.07.028also 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.