With the booming development of flexible and wearable electronics, their safety issues and operation stabilities have attracted worldwide attentions. Compared with traditional liquid electrolytes, gel polymer electrolytes (GPEs) are preferred due to their higher safety and adaptability to the design of flexible energy storage devices. This review summarizes the recent progress of GPEs with enhanced physicochemical properties and specified functionalities for the application in electrochemical energy storage. Functional GPEs that are capable to achieve unity lithium‐ion transference number and offer additional pseudocapacitance to the overall capacitance are carefully discussed. The smart GPEs with self‐protection, thermotolerant, and self‐healing abilities are particularly highlighted. To close, the future directions and remaining challenges of the GPEs for application in electrochemical energy storages are summarized to provide clues for the following development. Gel polymer electrolytes represent an attractive alternative to liquid electrolytes due to the superiorities of higher safety, better flexibility, and higher workability, which are promising for the use in electrochemical energy storage for the next‐generation flexible and wearable electronics. Their recent advancements, challenges, and perspectives are highlighted to provide guidance for the future study.