Recent research suggests that visual-verbal paired associate learning (PAL) taps a crossmodal associative learning mechanism involved in reading acquisition. However, evidence from children with dyslexia indicates that deficits in visual-verbal PAL are strongly linked to the verbal demands of the task. The research presented in this thesis had two overarching aims: first, to dissociate crossmodal and verbal demands in driving the PAL-reading relationship, and second, to assess the hypothesis that visual-verbal PAL plays a causal role in reading development. To address the first aim, a series of experiments examined the relationship between reading ability and PAL tasks differing in modality (crossmodal, unimodal) and output demand (visual, verbal). The results supported a verbal account of the PAL-reading relationship. In typically developing children and children with dyslexia, only tasks with a verbal output demand (i.e., visual-verbal PAL, verbal-verbal PAL) demonstrated a relationship with reading ability. In children with dyslexia, poor performance was isolated to difficulties learning novel phonological forms, rather than difficulties specific to crossmodal associative learning. Furthermore, the ability to learn novel phonological forms was found to fully explain visual-verbal PAL performance across reading abilities. In a final experiment, the causal role of visual-verbal PAL in reading development was assessed. The results of a longitudinal study from the start to the end of kindergarten showed that visual-verbal PAL measured in pre-readers did not predict reading ability at the end of kindergarten. Instead, PAL performance was influenced by learning to read.