In this research, two different jarosites generated by biological (bio-jarosite) and chemical (chem-jarosite) methods were used to study the uranium (U) removal efficiency and adsorption mechanism. The results showed that the maximum removal rate of U by bio-jarosite reached 77.4% and the U loading capacity was 43.4 mg/g, while the maximum removal rate was 67.2% and loading capacity was 33.6 mg/g for chem-jarosite under shaking conditions. SEM results showed that the surface of bio-jarosite is rougher than chem-jarosite, indicating a greater number of active sites were exposed on the bio-jarosite surface. Morphology would be one of the reasons why bio-jarosite has higher uptake capacity than that of chem-jarosite. These findings indicate that biogenerated jarosite is a great adsorbent for U remediation, but it was affected by bioleaching bacteria and pH. In addition, the bioleaching bacterium Sulfobacillus thermosulfidooxidans shows good potential as an adsorber of uranium.