The discharge of emulsion, cationic dyes, and heavy metals often coexists in wastewaters, greatly enhancing the difficulty of processing. In this work, we fabricated a nonswelling silica-poly(acrylic acid) (SiO2-PAA) composite through the surface modification of SiO2 using PAA to remove emulsion, cationic dyes, and heavy metal co-contaminants simultaneously. In the SiO2-PAA composite, PAA exists in a linear and divergent form rather than a network structure. Thus, SiO2-PAA can gain the nonswelling property, provide abundant carboxyl groups as the binding sites for removal of pollutants, which is an important advanced feature of PAA-based materials, and improve the potential of practical application. The characterization results of SiO2-PAA demonstrated that PAA was successfully grafted on SiO2. In a monocomponent system, SiO2-PAA exhibited excellent separation efficiency for cetyltrimethyl ammonium bromide (CTAB)-stabilized emulsion separation and admirable adsorption capacity of 758.6 and 178.6 mg/g for methylene blue (MB) and Cr(III). This finding was ascribed to the exposure of carboxyl groups in SiO2-PAA, which could increase the mass transfer efficiency. Importantly, the SiO2 PAA composite exhibited high efficiency in the simultaneous uptake of CTAB-stabilized emulsion, MB, and Cr(III) co-contaminants. Thus, given the simple fabrication, efficient emulsion separation, admirable adsorption capacity, and excellent reusability of SiO2-PAA, it exhibits striking potential for the efficient treatment of coexisting pollutants.