The adsorption behavior of Cr(III) and Cr(VI) ions onto laboratory-synthesized 2-line ferrihydrite was investigated under a batch method as a function of initial chromium concentration (0.1–1000 mg L−1) and pH (3.0 and 5.0). Moreover, the effect of the type of anion (chloride and sulfate) on Cr(III) adsorption was studied. The affinity of Cr(III) ions for the ferrihydrite surface depended on both the type of anion and pH of the solution and the maximum adsorption capacities decreased as follows: q (SO42−, pH 5.0) > q (SO42−, pH 3.0) > q (Cl−, pH 5.0) > q (Cl−, pH 3.0), and were found to be 86.06 mg g−1, 83.59 mg g−1, 61.51 mg g−1 and 40.67 mg g−1, respectively. Cr(VI) ions were bound to ferrihydrite in higher amounts then Cr(III) ions and the maximum adsorption capacity increased as the pH of the solution decreased and was 53.14 mg g−1 at pH 5.0 and 83.73 mg g−1 at pH 3.0. The adsorption process of Cr species was pH dependent, and the ions were bound to the surface of ferrihydrite by surface complexation. The Sips isotherm was the best-fit model to the results obtained from among the four isotherm models used, i.e., Freundlich, Langmuir, Dubinin-Radushkevich and Sips, indicating different adsorption centers participate in Cr uptake. In order to assess the bonding strength of the adsorbed chromium ions the modified BCR procedure, dedicated to the samples with a high iron content, was used. The results of the sequential extraction showed that Cr(III) ions were bound mainly in the immobile residual fraction and Cr(VI) ions were bound in the reducible fraction. The presence of Fe (oxyhydr)oxides in soil and sediments increases their adsorption capacity for Cr, in particular for hexavalent Cr in an acid environment due to their properties (high pHPZC).