A large amount of acidic wastewater was generated from the soil washing process. This study focuses on the capture for the radionuclide, especially cesium (Cs), in soil washing wastewater. We conducted the two-step process to reduce the amount of radioactive wastewater after soil washing using the coagulants and adsorbents in each step. We synthesized the adsorbent to capture Cs radionuclides in acidic wastewater (pH < 1). Based on the results, we found that the optimum ratio (NiFC:PAN) was 3.5:1 for the removal efficiency and strength of adsorbent. We compare the NiFC powder and NiFC-PAN for removal efficiency and separation of adsorbent after batch test, showing that the removal efficiency and separation of NiFC-PAN was lower and higher than NiFC power, respectively. We conducted the radioactive experiment to evaluate the satisfaction below release criteria (< 10 Bq·L−1, Cs), reporting that NIFC-PAN adsorbent meet the release criteria. These results showed that NiFC-PAN is promising adsorbent for Cs capture in strong acidic wastewater generated from soil washing and separation after capture process.