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Among various conducting polymers, polypyrrole(PPy) operating in aqueous electrolytes is a potential candidate for the use as soft actuators, or artificial muscles. But a considerable improvement in the performance of the PPy actuators is still required for successful applications. This book therefore aimed to get a better understanding of the processes associated with actuation mechanism of PPy actuators so as to improve their performance and explored a detailed understanding of the ionic motion and solvent transport during its actuation. A novel aspect of this book is the use of the unique physico-chemical environment of PPy to develop a more direct way of obtaining reliable values for the hydration numbers of cations in aqueous electrolytes and a detailed systematic investigation on the hydration number of metal ions in alkali metal, alkali earth metal and alkali rare earth metal chlorides electrolytes having different concentrations has also been included. At the last, significant advances on overall electro-chemo-mechanical performance of the PPy actuator with respect to primary solvation model of the counter ions were given in terms of speed of response and maximum strain.