Contamination of concrete at various nuclear power plants and spent nuclear fuel reprocessing facilities by radionuclides represents a significant problem for the world's nuclear power industries and nuclear waste management. The present publication summarizes the most recently published data on Electrokinetic Remediation (EK) of various concrete installations and advantageous effects of the combination of EK with different chelating agents. The specific aspects of decontamination of concrete and mortar surfaces are analyzed, such as: (a) effect of chelating agents (EDTA, citric acid), (b) effect of the zeta-potential (zeta) of concrete surface, (c) effects of sorption and complex formation equilibrium, and (d) specific advantages and problems of the electrokinetic decontamination process. The results of laboratory and in situ tests of chelating agent assisted EK removal of radionuclides are reported. It is demonstrated that the correct combination of EK with specific chelating agents can be effectively employed for decontamination of concrete surfaces.