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This work studies the Pb(II) removal onto bentonite clay modified by hexadecyl trimethyl ammonium bromide (HDTMA). Characterizations of the unmodified and modified materials were performed by using XRD, SEM, TG-DSC, FT-IR, and BET surface area analyses. Factors influencing the uptake of Pb(II) from aqueous solution, such as pH solution , ion strength, uptake time, adsorbent dosage, and initial Pb(II) concentration, were examined. The obtained results showed that bentonite clay was successfully modified by HDTMA, resulting in an increase in its surface area by about 70 %. The Pb(II) adsorption onto modified bentonite clay reached equilibrium at pH = 5.0 after 120 min. Studies within the isotherm and kinetic models demonstrated that the adsorption followed the Sips isotherm and pseudo-second-order kinetic models. The maximum monolayer adsorption capacity calculated from the Langmuir model at 30 °C was 25.8 mg/g, which is much higher than that obtained for the unmodified sample (18.9 mg/g). The FT-IR and TG-DSC analyses indicated that the formation of inner-sphere complexes plays a fundamental role in the mechanism of Pb(II) uptake onto HDTMA-bentonite clay. This mechanism of Pb(II) adsorption was further investigated, for the first time, by using the positron annihilation lifetime (PAL) and electron momentum (EMD) measurements. The PAL and EMD analyses indicated that the existence of Al and Si mono-vacancies in the HDTMA-bentonite should have essential contributions to the adsorption mechanism. In particular, we found a very interesting mechanism that the Pb(II) adsorption should occur inside the interlayer spaces of the HDTMA-bentonite. [Display omitted] • Bentonite clay was modified by HDTMA to enhance the Pb(II) removal. • The Langmuir monolayer adsorption capacity of HDTMA-modified bentonite was 25.8 mg/g. • The mechanisms of Pb(II) adsorption were studied via different analytical methods. • The formation of inner-sphere complexes played a major mechanism in the Pb(II) uptake. [ABSTRACT FROM AUTHOR]