This study enhanced the dye adsorption capacity and efficiency over Fe3O4@MOFs series composite adsorbents through enhancing the loading of MOFs. A multiple loading method was developed for controlling the loading percentage of MOFs in Fe3O4@MOFs series composite adsorbents, the values of which were calculated by the analysis of results of thermogravimetric analysis, X-ray diffraction, Fourier transform infrared spectroscopy, X-ray photoelectron spectroscopy, inductively coupled plasma mass spectrometry, Brunauer–Emmett–Teller, and vibrating sample magnetometry measurements. Dye adsorption test presented that an optimized adsorbent with enhanced adsorption capacity and adsorption efficiency could be achieved through enhancing the MOF loading in Fe3O4@MOFs series composite adsorbents.