We demonstrate that very stable hydrogels can be formed in aqueous potassium chloride solution by mixing a well-known gelator (guanosine, G) with a nongelator of similar structure (2,3',5'-tri-O-acetylguanosine, TAcG), and through a variety of characterization methods including rheology, small-angle neutron scattering, differential scanning calorimetry, and atomic force microscopy, we report substantial progress toward elucidating the factors that control the structure and stability of this fibrous gel system. The results suggest that the tailorability, long lifetime stability, and thermomechanical behavior of these gels derives from a reduction in the driving force toward crystallization with increased hydrophobic (TAcG) content, accompanied by a simultaneous decrease in fiber length and an increase in fiber width.