Metal nanoclusters (1-10 nm) have drawn great attention because of their potential applications including energy storage, catalysis, nanomedicine, and electronic devices. However, manufacturing ultrasmall metal nanoparticles at high concentrations in an unaggregated state is not a solved problem. Here, we report an aerosol-based thermal shock technique for in situ synthesis of well-dispersed metal nanoclusters in on-the-fly graphene aerosols. A rapid thermal shock to the graphene aerosol has been used to nucleate and grow the metal nanoclusters with subsequent quenching to freeze the newly formed nanoclusters in the graphene aerosol matrix. A characteristic time analysis comparison with the experiment shows that the nanocluster formation is governed by nucleation and subsequent surface growth and that the graphene retards coagulation, enabling unaggregated metal nanoclusters. The method is generic, and we show the formation of sub-10 nm Ni, Co, and Sn nanoclusters. This continuous aerosol-based thermal shock technique offers considerable potential for the scalable synthesis of well-dispersed and uniform metal nanoclusters stabilized within a host matrix. As an example of potential application, we demonstrate very favorable catalytic properties.