In our simulations, we observe a weak volume change (i.e., less than 4% for compression and 2% for stretching cases (see Supporting Information Figure ). A considerable volume change can affect the translational entropy of free counterions and change the fraction of condensed ions . If we can approximate the translational free energy per ion as the deformation-free volume available for ion diffusion at λ = 0, the translational free energy change with respect to the volume at the maximum compression, V λ could be written as ∆F ∼ k B T log(V 0 /V λ ). This leads to a translational energy change per ion ∆F ∼ 10 -2 k B T per ion. This change is significantly weaker than the energy that an ion can gain upon condensation, which is on the order of ∼ 0.1 -1k B T (see Supporting Information Figure . S4). Therefore, we conclude that the alterations in the fraction of condensed counterions cannot be due to the deformation-dependent swelling or shrinkage of the hydrogel but rather due to conformational changes of the individual chains composing the hydrogel. Finally, to confirm that the deformation-dependent condensation phenomenon that we observe does not depend on the calculation method used to distinguish condensed and free counterions, we calculate the radial distribution of counterions around each constituting various strain values. The distribution of counterions is obtained by counting the counterions within an imaginary cylindrical cell positioned around each PE chain of the hydrogel (see Figure . 3a) Once the counterion distribution is calculated as a function of the radial distance ρ, the cumulative number of counterions around the chains can be obtained by integrating the distribution data. In Figure. 3, we show the radial distributions and integrated distributions defined in Eq. 2 for the hydrogel chains aligned in the ẑ-direction. Consistent with the data in Figure . 2, the chain extension leads to an increase in the concentration of ions around the chains. For compressed and strongly stretched chains, on the other hand, we observe fewer counterions nearby the chains. Thus, the condensation patterns in Figure . 3 are qualitatively similar to the data shown in Figure . 2, suggesting that deformation-induced condensation alterations are not a side effect of the method used to determine the condensed counterions.