Adsorptive separation technologies have proven to be effective on organic contaminant removal in aqueous water. However, the breakthrough of contaminants is inevitable and can be at relatively low bed volumes, which makes the regeneration of spent adsorbents an urgent need. Electrochemically induced regeneration processes are given special attention and may provide ease of operation through in situ regeneration avoiding (i) removal and transport adsorbents, and (ii) avoiding use of hazardous chemicals (i.e., organic solvents, acids, or bases). Therefore, this review article critically evaluates the fundamental aspects of in situ electro-regeneration for spent carbons, and later discusses specific examples related to the treatment of emerging contaminants (such as per- and polyfluoroalkyl substances or PFAS). The fundamental concepts of electrochemically driven processes are comprehensively defined and addressed in terms of (i) adsorbent characteristics, (ii) contaminant properties, (iii) adsorption/regeneration driving operational parameters and conditions, and (iv) the competitive effects of water matrices. Additionally, future research needs and challenges to enhance understanding of in situ electro-regeneration applications for organic contaminants (specifically PFAS)-laden adsorbents are identified and outlined as a future key perspective.