Phenol contaminants are highly biotoxic and have become a global problem threatening the environment and human health. The objective of the present study was to develop a very efficient and easily recyclable adsorbent to remove phenol. A magnetic montmorillonite composite with organic co-intercalation was fabricated by a simple one-step co-precipitation method and exhibited excellent phenol removal. Two surfactants, cetyltrimethylammonium bromide (CTAB) and erucic acid amide (EA), were successfully co-intercalated into the interlayer of Ca-montmorillonite, and Fe3O4 nanoparticles were simultaneously decorated to obtain Fe3O4-CTAB/EA-montmorillonite composite (Fe3O4-C/E-Mnt). The morphology and structure of Fe3O4-C/E-Mnt composite were explored by using different techniques such as X-ray diffraction, Fourier-Transform infrared spectroscopy, X-ray photoelectron microscopy and so on. The adsorption capacity of Fe3O4-C/E-Mnt for phenol was investigated under various conditions including temperature, pH, contact time, various phenol concentrations, and adsorbent dosage. The results showed that Fe3O4-C/E-Mnt retained a lamellar structure of Ca-Mnt with mesopores. Its interlayer space, surface area, and pore volume were increased. The Fe3O4-C/E-Mnt composite exhibited a good adsorption capacity (31.45 mg·g–1) for phenol with a removal efficiency of 85.46% at optimized conditions. Moreover, the adsorbent still maintained 78.32% of the adsorption capacity after five cycles. The adsorption test data of Fe3O4-C/E-Mnt followed the pseudo-second order kinetic model and the Langmuir model. The adsorption was a spontaneous, exothermic, entropy-decreasing process, and a possible adsorption mechanism of Fe3O4-C/E-Mnt was finally proposed.