Herein, we report the synthesis of double-shelled periodic mesoporous organosilica nanospheres/MIL-88A-Fe (DSS/MIL-88A-Fe) composite through a hydrothermal method. To survey the structural and compositional features of the synthesized composite, a variety of spectroscopic and microscopic techniques, including FT-IR, XRD, BET, TEM, FE-SEM, EDX, and EDX-mapping, have been employed. A noteworthy point in this synthesis procedure is the integration of MOF with PMO to increase the adsorbent performance, such as higher specific surface area and more active sites. This combination leads to achieving a structure with an average size of 280 nm and 1.1 μm long attributed to DSS and MOF, respectively, microporous structure and relatively large specific surface area (312.87 m2/g). The as-prepared composite could be used as an effective adsorbent with a high adsorption capacity (250 mg/g) and quick adsorption time (30 min) for the removal of Pb2+from water. Importantly, DSS/MIL-88A-Fe composite revealed acceptable recycling and stability, since the performance in Pb2+removal from water remained above 70% even after 4 consecutive cycles.