A direct, all-aqueous electrospinning method for fabricating degradable nanofibrous hydrogel networks is reported in which hydrazide and aldehyde-functionalized poly(oligoethylene glycol methacrylate) (POEGMA) polymers are simultaneously electrospun and cross-linked. The resulting networks are spatially well-defined, mechanically stable (both dry and wet), and offer extremely fast swelling responses, suggesting potential utility as smart hydrogels and tunable tissue engineering matrices.