Prediction error is known to enhance priming effects for familiar syntactic structures; it also strengthens the formation of new declarative memories. Here, we investigate whether violating expectations may aid the acquisition of new abstract syntactic structures, too, by enhancing memory for individual instances which can then form the basis for abstraction. In a cross-situational artificial language learning paradigm, participants were exposed to novel syntactic structures in ways that either violated their expectations (Surprisal group) or that conformed to them (Control group). Results from a delayed post-test show that participants in the Surprisal group developed stronger representations of the structures’ form-meaning mappings and were better able to generalize them to new instances, relative to the Control group.