Specifically, we selected DNA-triggered spontaneous and non-specific aggregation of AuNPs as the positive feedback and their heat-induced redispersion as the negative feedback mechanism (Figure ). Here, the aggregation-induced redshift in the extinction of AuNPs increases the lightharvesting properties of the system in the assembled state under non-periodic irradiation with a laser that serves as the energy source. This increased light absorption produces photothermal heating that results in the melting of DNA and ultimately, the disassembly of AuNPs (light-induced asymmetry, see Figure ). The time delay was introduced through thermal hysteresis which is a typical feature of selfassembling NP. Under suitable experimental conditions (base temperature and laser power), we observed that the local heating by AuNPs, coupled with thermoresponsive selfassembly could induce forces (thermal buoyancy) that resulted in hydrodynamic oscillations in our system. Although the oscillations could be observed for a range of temperatures and laser powers, they were sensitive to the initial conditions of the experiment. Our system thus exhibits hierarchical features, where, angstrom scale molecular components control the assembly of NPs, which finally translates into mm-scale oscillating hydrodynamic flows (Figure ). These oscillating hydrodynamic flows have potential applications in the fields of chemical computing, fuzzy logic, and artificial neuron network models. To assure the increase of extinction at the NIR spectral range (∼808 nm, resonant with the laser light source) we selected a mixture of DNA-coated gold nanospheres (AuSs, diameter = 28.2 ± 2.4 nm, Figure ) and gold nanorods (AuNRs, length = 54.5 ± 4.8 nm, width = 18.6 ± 1.5 nm, Figure ). The native ligands were place exchanged with thiolated DNA (see Figure ) using the freeze-drying method. For more details on the synthesis and ligand exchange process, see Section S1.2, and S1.3 in the SI. These DNA-coated AuNPs underwent aggregation in the presence of complementary DNA (aggregating DNA) under high ionic strength (∼200mM NaCl) due to the salting-out effect (Figure ). Note that unary systems based on either AuSs or AuNRs were unable to exhibit the desired spectral shift upon aggregation. Although a dispersion of AuSs exhibits redshifts during aggregation, their photothermal heating is relatively poor (weak negative feedback) (see Figure , S5). Conversely, AuNRs despite having high photothermal heating abilities, often display minor redshifts due to more stable side-to-side assembly configurations (see Figure ). By mixing and assembling AuNRs and AuSs, unstructured aggregates form that exhibit reliable and consistent redshifts along with high photothermal heating abilities, thereby fulfilling both important criteria for choreographing an oscillating response.