The induced aggregation of the xanthenedye rho-damineB (RhB) on metal oxide centers belonging to the highly symmetric surfaces of precise nanoscale templates with Keplerate (Mo 132 )o rtoroidal (Mo 138 )s tructures has been studied. With the joint use of the Langmuir isotherma nd full Stern-Volmer models, the thermodynamic reasons for dye adsorption on the nanocluster surface, such as amixture of monomer,H -aggregate (H-dimer), and J-aggregate forms (which can coexist or switch one into another under the exact conditions), were established:t his was shown through UV/Vis and fluorescence spectroscopies. By using the frame-work of the excitonm odel, it is shownt hat the angle( a)b etweent he transition dipole moments of RhB is very sensitive to surface strain inside the dye sub-monolayer.A saresult, it is possible to switch from H-to J-aggregates by the postfunctionalization of polyoxometalate (POM)-RhB associates by the surfactant bilayer shell, which allows the surface strain to grow.R ecommendations are provided for managing the appearance of H-or J-aggregates on metal oxide (or polyelectrolyte) surfacesd uring photovoltaico rb ioimaging applications.[a] V. Fazylova, N. Shevtsev,S .M ikhailov, Prof. [b] G. Kim Institute of Organic Synthesis Ural Branch of the Russian Academyo fSciences 22 AkademicheskayaS t.,6 20990 Ekaterinburg (Russia) Supporting information and the ORCID identification number(s) for the author(s) of this article can be found under: https://doi.