In this work, new imidazolium silica-ionic liquids doped with magnetite nanocomposites are prepared for use in the field of water purification owing to their unique properties, which can be manipulated by an external magnetic field. A silane precursor based on aminopropyltriethoxysilane (APTS) condensed with p-hydroxybenzaldehyde and glyoxal in an acetic acid solution is used to prepare disiloxyimidazolium ionic liquid (SIMIL). The silica composite (Si-IL) and silica-coated magnetite (Fe 3 O 4 -Si-IL) composites are prepared using the sol-gel technique. The chemical structures, morphologies, crystalline lattice structures, thermal stabilities, surface charges, surface areas, particle sizes, and magnetic characteristics of Fe 3 O 4 -Si-IL and Si-IL are investigated. The Fe 3 O 4 -Si-IL and Si-IL nanocomposites show excellent chemical adsorption capacities as 653 and 472 mg g −1 , respectively, during times ranging 90 to 110 min when they are used as adsorbents to remove Congo red (CR) dye as a water pollutant.Nanomaterials 2020, 10, 71 2 of 19 and integrate the merits of functional nanoparticles and vary the solid hosts of the large sizes of materials [8][9][10]. Although magnetic nanocomposites have achieved excellent results with adsorption and reuse for different cycles in the field of water treatment, some research challenges exist for their application to remove some pollutants such as toxic radioactive metals and organic and agricultural pollutants [9].The concept of a synergistic combination of two nanoparticles into a larger one has become one of the proposed synthetic techniques used to design advanced nano-adsorbents for water treatments [11][12][13][14]. Most of these materials are based on mesoporous silica-based adsorbents [15][16][17]. The large pore sizes, high specific area, good thermal and chemical stability, low manufacture cost, and excellent selectivity towards specific pollutants elect the ordered mesoporous silica composites as excellent adsorbents for water purification and treatment [17][18][19]. Highly dispersed and magnetic silica nanoparticles with large-scale chemical or sonochemical synthesis methods have been reported [20][21][22][23][24][25].With the large amount of literature available for the production of magnetic silica nanoparticles and with research still being published, perhaps some of the biggest challenges to overcome regard the production of greener selective magnetic silica nano-adsorbents for removal of organic pollutants; these are still a problem facing researchers. Organic cationic and anionic salts based on imidazolium, pyridinium, and quaternary ammonium cations which have been designated as ionic liquids (ILs) are widely used as greener extraction solvents for seawater desalination and industrial water and activated sludge treatments [26][27][28][29]. Poly (ionic liquid) (PIL) nanoparticles are used as flocculants for water purification [28], and hydrophobic PILs have been used for the selective separation of methylene blue (MB) dye and chromium ions from water [3...