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Efficient removal of radioactive cesium from complex wastewater is a challenge. Unlike traditional precipitation and hydrothermal synthesis, a novel vast specific surface area adsorbent of copper hexacyanoferrates named EA-CuHCF was synthesized using a one-pot solvothermal method under the moderate ethanol media characterized by XRD, SEM, EDS, BET, and FTIR. It was found that the maximum adsorption capacity towards Cs+ was 452.5 mg/g, which is far higher than most of the reported Prussian blue analogues so far. Moreover, EA-CuHCF could effectively adsorb Cs+ at a wide pH range and low concentration of Cs+ in geothermal water within 30 minutes, and the removal rate of Cs+ was 92.1%. Finally, the separation factors between Cs+ and other competitive ions were higher than 553, and the distribution coefficient of Cs+ reached up to 2.343 × 104 mL/g. These properties suggest that EA-CuHCF synthesized by the solvothermal method has high capacity and selectivity and can be used as a candidate for Cs+ removal from wastewater.