The controlled structuring of liquids into arbitrary shapes can be achieved in biphasic liquid media using the interfacial assemblies of nanoparticle surfactants (NP-surfactants), that consist of a polar nanoparticle "head group" bound to one or more hydrophobic polymer "tails". The nonequilibrium shapes of the suspended liquid phase can be rendered permanent by the jamming of the NP-surfactants formed and assembled at the interface between the liquids as the system attempts to minimize the interfacial area between the liquids. While critical to the structuring process, little is known of the dynamic mechanical properties of the NP-surfactant monolayer at the interface as it is dictated by the characteristics of the component, including NP size and concentration and the molecular weight and concentration of polymers bound to the NPs. Here we provide the first comprehensive understanding of the dynamic mechanical character of two-dimensional NP-surfactant assemblies at liquid/liquid interfaces. Our results indicate that the dynamics of NP-polymer interactions are self-regulated across multiple time scales and are associated with specific mesoscale interactions between self-similar and cross-complementary components. Furthermore, the mechanical properties of the NP-surfactant monolayer are tunable over a broad range and deterministic on the basis of those component inputs. This control is key to tailoring the functional attributes of the reconfigurable structured liquids to suit specific applications.