NH 2 –MIL–101(V), an amine-functionalized vanadium-based metal–organic framework (MOF) material, was successfully synthesized using a solvothermal strategy. The obtained material was characterized by X-ray diffraction (XRD), N 2 adsorption–desorption isotherms, Fourier transformed infrared spectroscopy (FTIR), X-ray photoelectron spectroscopy (XPS), scanning electron microscope (SEM) and transmission electron microscopy (TEM) techniques. The CO 2 and N 2 adsorption properties of the material were measured using the Micromeritics ASAP 2020 apparatus under ambient conditions. Compared to the previously reported method for synthesizing this MOF, we performed synthesis under a lower reaction temperature. Despite this, pure-phase NH 2 –MIL–101(V) nanocrystals with diameters of 40–60 nm were achieved. The synthesized sample had a large specific surface area (2340 m 2 /g), denoting a substantial enhancement to the literature value of the corresponding analogue. In addition, the NH 2 –MIL–101(V) possessed a high CO 2 uptake of 1.9 mmol/g at 25 °C and a pressure of 100 kPa and exhibited high CO 2 /N 2 selectivity as well as moderate CO 2 isosteric heat of adsorption.