In this study, a metal-organic framework (MOF) material NH2-MIL-101(Fe) was synthesized using the solvothermal method, and characterized by X-ray diffraction (XRD), Fourier transform infrared spectroscopy (FT-IR), UV-visible spectrophotometry, field-emission scanning electron microscopy (FE-SEM), energy dispersive X-ray spectroscopy (EDS), transmission electron microscopy (TEM), and surface area measurements. The XRD pattern of the synthesized NH2-MIL-101(Fe) was similar to the previously reported patterns of MIL-101 type materials, which indicated the successful synthesis of NH2-MIL-101(Fe). The FT-IR spectrum showed the molecular structure and functional groups of the synthesized NH2-MIL-101(Fe). The UV-visible absorbance spectrum indicated that the synthesized material could be activated as a photocatalyst under visible light irradiation. FE-SEM and TEM images showed the formation of hexagonal microspindle structures in the synthesized NH2-MIL-101(Fe). Furthermore, the EDS spectrum indicated that the synthesized material consisted of Fe, N, O, and C elements. The synthesized NH2-MIL-101(Fe) was then employed as an adsorbent and photocatalyst for the removal of Indigo carmine and Rhodamine B from aqueous solutions. The initial 30 min of adsorption for Indigo carmine and Rhodamine B without light irradiation achieved removal efficiencies of 83.6% and 70.7%, respectively. The removal efficiencies thereafter gradually increased with visible light irradiation for 180 min, and the overall removal efficiencies for Indigo carmine and Rhodamine B were 94.2% and 83.5%, respectively. These results indicate that the synthesized MOF material can be effectively applied as an adsorbent and photocatalyst for the removal of dyes.