The assembly of monomers that feature dynamic non-covalent interactions furnishes supramolecular polymers. Stimuli that weaken the interactions between the monomers can trigger a temporary disassembly of the building blocks, which imparts the materials with useful responsive functionalities. In this presentation, we report on the use of supramolecular self-assembly to create polymer films that combine desirable responsive functionalities with tailored mechanical properties. Thus, a recently developed approach will be discussed that allows blending two building blocks to achieve superior mechanical properties. The ability to combine the building blocks in any ratio enables the fabrication of polymer films with a spatially modulated mechanical behavior, effectively mimicking the anisotropic properties of more complex natural materials. Moreover, this presentation will also discuss approaches toward nanoparticle composite and highlight recently developed materials that display defined optical signals upon mechanically deformation.