Using batch method, the adsorption of thallium(I) ions from aqueous solutions on eucalyptus leaves powder, as a low cost adsorbent, was studied. The effect of various modification of considered adsorbent on the adsorption percentage of Tl(I) is an important feature of this study. The results showed that the unmodified and acidic modified adsorbent are the poor adsorbents for the Tl(I) ions while basic modified adsorbent is a suitable adsorbent. Also, the effect of some experimental conditions such as solution initial pH, agitation speed, contact time, sorbent dosage, temperature, particle size, and thallium initial concentration was studied. The results showed that the adsorption percentage depends on the conditions and the process is strongly pH-dependent. The satisfactory adsorption percentage of Tl(I) ions, 81.5%, obtained at 25 ± 1°C. The equilibrium data agreed fairly better with Langmuir isotherm than Freundlich and Temkin models. The value of qm that was obtained by extrapolation method is 80.65 mg g−1. Separation factor values, RL, showed that eucalyptus leaves powder is favorable for the sorption of Tl(I). The negative values of ΔH0 and ΔS0 showed that the Tl(I) sorption is an exothermic process and along with decrease of randomness at the solid–solution interface during sorption, respectively.