Peptide nanotubes were used as templates for the growth of poly(ethylene glycol) diacrylate-based nanoscale hydrogels via photopolymerization. A Rose Bengal di-amine derivative comprised of a photoactivator and coinitiator within the same molecule was used as the photoinitiator to increase photopolymerization efficiency. The nanotubes were covalently bound to the protein BSA before formation of the hydrogels. We also examined the photopolymerization efficiency in reactions involving nanotubes in the absence of BSA. Although photopolymerization occurred efficiently under both conditions, higher yields of highly crosslinked nanostructures were obtained for the protein bound nanotube-PEGDA hydrogels. It was observed that the swelling ratios were also dependent upon whether or not BSA was bound to the nanotubes before photopolymerization. The thermal properties of the nanocomposite hydrogels were investigated using differential scanning calorimetry analyses and the morphologies were examined using TEM, SEM, and AFM analyses. Such nanocomposites prepared by low cost, mild methods could be extremely efficient for the in situ preparation of three-dimensional arrays of peptide nanotube grafted hydrogels.