The aim of this study is to investigate the sorption/ion exchange of radioactive nuclides such as Cs+ and Sr2+ by synthetic Na-micas. In order to prepare Na-micas, two natural micas (phlogopite and biotite) were used as precursor materials. XRD, SEM, and EDS analyses were used to examine material characterization of synthetic Na-micas. Analyses of materials revealed that Na-micas were successfully obtained from natrual micas by K removal treatment. On the other hand, single solute (Cs or Sr) and bi-solute (Cs/Sr) sorption experiments were carried out to determine sorption capacity of Na-micas for Cs and Sr under different pH and ionic strength conditions. Uptake of Cs and Sr by micas in bi-solute system was lower than in single-solute system. Additionally, Langmuir and Langmuir competitive models were applied to describe sorption isotherm of Na-micas. bi-solute system was well described by Langmuir competitive models. For the results obtained in this study, Na-micas could be promising sorbents to treat multi-radioactive species from water and groundwater.