In this work, we demonstrate that monodispersed hollow mesoporous organosilica nanospheres (MONs) and yolk-shell MONs possessing controlled core cavity and mesoporous shell is successfully synthesized through a one-pot approach, which involves co-condensation of 3-aminopropyltriethoxysilane and 1,2-bis(triethoxysilyl)ethane templated by lauryl sulfonate betaine and sodium dodecyl benzenesulfonate. The MONs present an open mesoporosity, hollow cavity with a morphology tailored by the various core templates, and high surface area (328 m2/g). In addition, the composition of the hollow MONs could be further tuned through the same approach. The as-prepared hollow MONs as adsorbent deliver an enormous adsorption capacity (414 mg/g) towards the removal of Pb2+ from water solution. Importantly, the prepared hollow MONs present acceptable recycling and stability, since the performance in Pb2+ removal from water remains above 80 % even after 5 consecutive cycles. The adsorption of Pb2+ on hollow MONs follows the pseudo-second-order mechanics and Langmuir isotherm models. The results confirm hollow MONs exhibit considerable promise for the remarkably efficient separation of Pb2+ ions in water solution.