Synthetic hydrogel systems are promising long-term candidates for therapeutic use as vitreous substitutes. To improve the swelling and mechanical properties of existing synthetic substitutes for the natural vitreous, we incorporate charges and fibrous structures. Using dynamic light scattering, rheology, and swelling techniques we show in vitro that synthetic copolymers of methacrylic acid (MAA), methylacrylamide (MAm), and bismethacryloylcystamine (BMAC) cross-linked with gellan match the water content, transport properties, and dynamic response of the natural vitreous better than previously proposed synthetic substitutes.