Magnetic metal-organic framework composites (MFCs) were prepared in water at room temperature through a simple, low-cost and green strategy only by employing organic salts as anionic linker sources. Aminofunctionalized MFCs (MFC-N) with different amino group contents were successfully prepared by varying the ratio of disodium of 2-aminoterephthalic (NH2-Na2 BDC)/terephthalic acid (Na2BDC). The prepared nanoscale MFC-N-X (X represents the percentage of NH2-Na2BDC, i.e., X = 0, 50, and 100) showed high surface area, large pore volume, excellent magnetic response, and good water and thermal stability. Among these prepared MFC-N-X, MFC-N-100 exhibited the highest adsorption capacity of 358 mg g(-1) for methylene blue (MB) and 71 mg g(-1) for As(V) due to its porous structure and abundant amino groups. The prepared MFC-N-100 was successfully applied to remove MB and As(V) from different water samples (tap water, lake water, and domestic sewage) with a high removal efficiency and a rapid separation of the sorbent from solution, demonstrating the great application potential of the prepared MFC-N-100 as a fascinating adsorbent for removal of dyes or metal ions from different water samples.