Periodic mesoporous organosilica nanoparticles (PMO SiNPs) were developed for the targeted capture of specific volatile organic compounds (VOCs). The removal kinetics for adsorbing VOCs were fast and the maximum removal could be achieved within less than 30 min. PMO SiNPs removed >99% of VOCs at a low sorbent dose (i.e. >0.5 mL analyte per g PMO SiNPs). They also showed good recyclability and maintained reasonable removal efficiencies after five cycles (i.e. 77% and 65% for hexanal and butyric acid vapors, respectively).