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Paired-associate learning is a dynamic measure of the ability to form new links between two items. This study aimed to investigate whether paired-associate learning ability is associated with success in orthographic learning, and if so, whether it accounts for unique variance beyond phonological decoding ability and orthographic knowledge. A group of 63 children ages 8–10 completed an orthographic learning task and three types of paired-associate learning task: visual–visual, visual–verbal, and verbal–verbal. The results showed that both visual–verbal and verbal–verbal (but not visual–visual) paired-associate learning ability were associated with success in learning the spellings of novel words. Moreover, hierarchical regression analyses showed that visual–verbal paired-associate learning predicted orthographic learning even after phonological decoding skill and existing orthographic knowledge had been accounted for. We propose that paired-associate learning ability may be one of the underlying mechanisms of orthographic learning, facilitating the connection between the phonology and orthographic representation of a word.