In this research, an organobentonite (HDTMA-BT) was prepared by modifying a jordanian bentonite (BT) with hexadecyltrimethylammonium bromide. By means of in situ free radical polymerization in THF with AIBN as the initiator, this organobentonite is used to prepare the polymethylmethacrylate-bentonite (PMA-HDTMA-BT) nanocomposite. Scanning electron microscopy (SEM), x-ray diffraction (XRD), energy dispersive spectrometer (EDS) and Fourier transform infrared (FTIR) spectroscopy were used to characterize both HDTMA-BT and PMA-HDTMA-BT. Those adsorbents were used in a batch process to remove Pb(II), Cr(III) ions, and p-chlorophenol (PCP) from aqueous solution. Investigated factors included adsorbent dosage, initial pH solution, contact time, and temperature. Adsorption data more fitted the Langmuir and D-R isotherms than the Freundlich isotherm. The maximum adsorption capacities, qmax, obtained from the Langmuir adsorption isotherm were 172.414 mg/g, 303.030 mg/g, 10.020 mg/g, 25.641 mg/g, 76.336 mg/g, and 163.934 mg/g for Pb/HDTMA-BT, Pb/PMA-HDTMA-BT, Cr/HDTMA-BT, Cr/PMA-HDTMA-BT, PCP/HDTMA-BT, and PCP/PMA-HDTMA-BT, respectively. The results on adsorption were found to be well-fit by the pseudo-second order kinetics model. The uptake of Pb(II), Cr(III) ions, or PCP onto HDTMA-BT and PMA-HDTMA-BT nanocomposite was primarily regulated by intraparticle diffusion, but boundary layer diffusion also took place in the adsorbate-adsorbent system. pH and temperature significantly influenced the adsorption process and negative values of suggest that the adsorption process was spontaneous and feasible.