1) GHK, QK, and HepIII were applied in solution either directly to hMVECs or to MSCs to elicit production of conditioned medium, which was then applied to hMVECs. hMVEC network formation was assessed to select a peptide for further use. 2) In parallel, a library of viscoelastic or elastic alginate hydrogels were created with varying crosslinker concentrations to produce gels of varying moduli. 3) The effect of all combinations of peptide content, viscoelasticity, and stiffness on the ability of MSCs to promote hMVEC network formation and undergo osteogenic differentiation was assessed in a high-throughput experiment. 4) From this screen, one formulation was selected for in vivo studies.