The potential application of aggregates of nanoparticles for high-speed flow diagnostics is investigated. Aluminum nanoparticles around 10 nm in diameter are produced by spark discharge in argon gas. Through rapid coagulation and oxidation, aggregates of small effective density are formed. They are characterized by microscopy and their aerodynamics and optical properties are theoretically evaluated. The performance of the aggregates is experimentally investigated across an oblique shock wave in a supersonic wind tunnel of 3 × 3 cm 2 cross-section at Mach 2. Particle image velocimetry is used to quantify the time response of the aggregates. The investigations are also carried out on compact titanium agglomerates to provide a base for comparison. The results yield a relaxation time of 0.27 μs for the nanostructured aluminum aggregates, which is an order of magnitude reduction with respect to the compact titanium nanoparticles. This work demonstrates the applicability of nanostructured aggregates for laser-based diagnostics in supersonic and hypersonic flows.