Ionic polymer-metal composites (IPMCs) consist of a perfluorinated ionomer membrane (usually Nafion® or Flemion®) plated on both faces with a noble metal such as gold or platinum and neutralized with a certain amount of counterions that balance the electrical charge of anions covalently fixed to the backbone ionomer. IPMCs are electroactive materials with potential applications as actuators and sensors. Their electrical-chemical-mechanical response is dependent on the cations used, the nature and the amount of solvent uptake, the morphology of the electrodes, the composition of the backbone ionomer, the geometry and boundary conditions of the composite element, and the magnitude and spatial and time variation of the applied potential. With water as the solvent, the applied electric potential must be limited to less than 1.3 V at room temperature, to avoid electrolysis. Moreover, water evaporation in open air presents additional problems. These and related factors limit the application of IPMCs with water as the solvent. We present the results of a series of tests on both Nafion- and Flemion-based IPMCs with ethylene glycol, glycerol, and crown ethers as solvents. IPMCs with these solvents have greater solvent uptake and can be subjected to relatively high voltages without electrolysis. They can be actuated in open air for rather long time periods, and at low temperatures. They may be good actuators when high-speed actuation is not necessary. In addition, their slow response in open air allows direct observation of the physical characteristics of the cathode and anode surfaces of a cantilever during actuations. This can provide additional clues for unraveling the underpinning micromechanisms of their actuation. Remarkably, solvents are found to have profound effects on the nature of the IPMCs’ actuation. For example, Nafion-based IPMCs in Li+ form show very small back relaxation when hydrated, but extensive back relaxation with all other solvents that we have considered. On the other hand, the same membrane in the K+ form has extensive back relaxations when solvated with water, or ethylene glycol, or glycerol, but none with 18-Crown-6.