A study was conducted to apply a number of spectroscopic techniques to N-fluorenymethoxycarbonyl diphenylanine (Fmoc-FF) gel, constructing a molecular model based on the data obtained comprising a new nanocylinderical molecular architecture of π interlocked β-sheets. The viscoelastic properties of the gels were assessed using oscillatory rheology. Circular dichroism (CD) was also used, to investigate the backbone orientation of the dipeptide within the hydrogel. The model was constructed using the HyperChem program, while the Amber forcefield was used to energy minimize the molecular structures formed in the program. Mechanical properties were carried out on a strain-controlled rheometer, using a cone-plate geometry. The dynamic moduli of the hydrogel were measured as a function of frequency between 0.01 and 100 Hz. A solvent trap was used, while the atmosphere within, was saturated with a cup of water, to keep the sample hydrated.