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The Flory‐Huggins binary interaction parameter and its enthalpy and entropy parts were experimentally determined for polyelectrolyte hydrogels based on poly(acrylic) acid (PAAc) and poly(methacrylic) acid (PMAc) with various mono‐ and divalent counterions. It was shown that water is a poor solvent for acrylic and methacrylic polyelectrolyte hydrogels, as the binary interaction parameter is around 0.8 for mono‐ and 0.6 for divalent counterions. The type of counterion affects the enthalpy‐interaction parameter and according to its increase in PAAc gels, counterions can be placed in the following order: Li+

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