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Polyelectrolyte complexes (PECs) are highly tunable materials that result from the phase separation that occurs upon mixing oppositely charged polymers. Over the years, they have gained interest due to their broad range of applications such as drug delivery systems, protective coatings, food packaging, and surface adhesives. In this review, we summarize the structure, phase transitions, chain dynamics, and rheological and thermal properties of PECs. Although most literature focuses upon the thermodynamics and application of PECs, this review highlights the fundamental role of salt and water on mechanical and thermal properties impacting the PEC's dynamics. A special focus is placed upon experimental results and techniques. Specifically, the review examines phase behaviour and salt partitioning in PECs, as well as different techniques used to measure diffusion coefficients, relaxation times, various superpositioning principles, glass transitions, and water microenvironments in PECs. This review concludes with future areas of opportunity in fundamental studies and best practices in reporting.