Our recent review describes the characteristics of a "stimuli-responsive material". Static systems (and static stimuli-responsive materials) undergo an irreversible transition from one local energy minimum to another or by shifting between different equilibria due to alterations in the parameters that define these equilibria. "Dynamic systems" are distinguished by their reliance on external stimuli to keep them out of equilibrium. Adaptive materials, being a broader term, exhibit specific responses to external stimuli, enabling them to reversible transition between equilibrium states, between equilibrium and non-equilibrium states, or between multiple non-equilibrium states. In the previous research, we presented the formation of the air-water interfacial adaptive system with FexOy@SiO2NPs capped with poly(N-isopropyl acrylamide) (ligand -PNIPAM, particles -PSiFe) as a building block. We provided data, an explanation of phenomena observed in the system, and an efficient deposition method for such hydrophilic nanomaterials on the water surface. Thermoresponsive PSiFe showed different behavior in two temperature regimesbelow and above the lower critical solution temperature (LCST) due to the changes in polymer chains capped on the surface of the nanoparticles. Extended PNIPAM at lower temperatures caused fractal aggregation and increased the interfacial area per nanoparticle in Langmuir layers. The results indicated nanoparticles' Janus-like conformation as the most probable, with polymeric ligands being "open" below and "closed" above the water surface. On the contrary, the conformation remained more anisotropic and fully closed at higher temperatures. No interdigitation and no internanoparticulate bonds between PNIPAM ligands were observed. The most exciting observation was that the films were more compact and ordered at a higher temperature. The surface pressure decreased at a higher temperature, i.e., behaved oppositely to classical systems.