A novel in situ method for measurement of mass concentration of nanoparticles (NPs) formed in flames is proposed. In this method, the deposition rate of NPs collected by a molecular beam sampling system is measured by quartz-crystal microbalance (QCM). It is the only existing method which allows direct measurement of NP mass concentration profiles in flames. The feasibility of the method was demonstrated by studying iron oxide NP formation in low-pressure methane/oxygen/nitrogen flames doped with iron pentacarbonyl. The system was tested under fuel-lean and fuel-rich flame conditions. Good agreement between measured QCM deposition rates and their estimations obtained by the transmission electron microscopy analysis of samples collected from the molecular beam has been demonstrated. The sensitivity of the method is comparable to that of particle mass spectrometry (PMS). Combination of the QCM technique with PMS and/or optical measurements can provide new qualitative information which is important for elucidation of the mechanisms governing the NP flame synthesis.