In this work, kaolinite modified with zero-valent iron was synthesized and used as a sorbent for Pb(II) and Mo(VI) removal from aqueous solutions. The obtained material was characterized by X-ray diffraction (XRD) and Fourier transform infrared (FTIR) spectroscopy. The methods revealed successful modification by the Fe0 particles precipitation on the surface of well-ordered kaolinite. The sorption experiment results showed a significant increase of sorption capacity in relation to the raw kaolinite. The kaolinite with 25% content of Fe0 was found to be the best material for Pb(II) and Mo(VI) removal, resulting in approximately 500 mmol·kg−1 and 350 mmol·kg−1 sorption, respectively. The possible mechanisms responsible for metals’ removal were identified as reduction by Fe0 ‘core’ and adsorption on the iron hydroxides ‘shell’. The study indicated that the obtained material is capable of efficient Pb(II) and Mo(VI) removal and may be an interesting alternative to other methods used for heavy metals’ removal.