Expanding the toolkit of modular and functional synthetic material systems for biomimetic extracellular matrices (ECMs) is needed for achieving more predictable and characterizable cell culture. In the present study, we engineered a synthetic hydrogel system incorporating poly(γ-propargyl- l -glutamate) (PPLG), an N -carboxy anhydride polypeptide with a unique α-helical secondary structure. PPLG macromers were cross-linked into poly(ethylene glycol) (PEG) networks to form hybrid polypeptide-PEG hydrogels. We compared the properties of PPLG-PEG to systems where the PPLG macromers were replaced with 8-arm PEG or poly(γ-propargyl- d , l -glutamate) (PPDLG), which has a flexible random-coil conformation. We evaluated each hydrogel system as synthetic ECMs for two-dimensional (2D) endothelial cell culture. Cells on PPLG-PEG displayed superior attachment and spreading at comparable adhesion ligand incorporation concentrations, demonstrating the unique benefit of combining the more rigid and hydrophobic α-helical PPLG within the more flexible and hydrophilic PEG matrix. The modular PPLG macromer is a promising building block for developing other types of PPLG-based hydrogels with favorable and tunable properties. Jump To The Supporting Information is available free of charge at https://pubs.acs.org/doi/10.1021/acs.biomac.9b01297 . GPC traces, NMR spectra, circular dichroism spectra, adhesive peptide incorporation efficiency, cryo-TEM images, volumetric swelling ratios and elastic moduli, plots of cell roundness and cell area coverage as a function of actual peptide concentrations, calculations of average mesh size and average molecular weight between cross-links ( PDF ) pdf bm9b01297_si_001.pdf (749.77 kb) Terms & Conditions
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