Peptide 1 with an Aβ42 amyloid nucleating core and a photodimerizable 4-methylcoumarin moiety at its N terminus demonstrates the step-wise self-assembly in water to form nanoparticles, with eventual transformation into 1D nanofibers. Addition of γ-cyclodextrin to 1 with subsequent irradiation with UV light at 320 nm resulted in morphological conversion to free-standing 2D nanosheets mediated by the host–guest interaction. Mechanical agitation of the 1D and 2D nanostructures led to seeds with narrow polydispersity indices, which by mediation of seeded supramolecular polymerization found seamless control over the dimensions of the nanostructures. Such structural and temporal control to differentiate the pathway was exploited to tune the mechanical strength of hierarchical hydrogel materials. Finally, the dimensional characteristics of the positively charged peptide fibers and sheets were envisaged as excellent exfoliating agents for inorganic hybrid materials, for example, MoS2.