Hydrogels are used widely for exploratory tissue engineering studies. However, currently, no hydrogel systems have been reported which exhibit a wide range of elastic modulus without changing precursor concentration, identity, or stoichiometry. Herein, ester- and amide-based poly(ethylene glycol) (PEG) eoxime hydrogels with tunable moduli (similar to 5-30 kPa) were synthesized with identical precursor mass fraction, stoichiometry, and concentration by varying the pH and buffer concentration of the gelation solution, exploiting the kinetics of oxime bond formation. The observed modulus range can be attributed to increasing amounts of network defects in slower forming gels, as confirmed by equilibrium swelling and small-angle neutron scattering (SANS) experiments. Finally, human mesenchymal stem cell (hMSC) viability was confirmed in these materials in a 24-h assay. While this was only an initial demonstration of the potential utility, the controlled variation in defect density and modulus is an important step forward in isolating system variables for hypothesis-driven biological investigations. (c) 2018 Elsevier Ltd. All rights reserved.