In this study, we examined the learning of letter-speech sound correspondences within an artificial script and performed an experimental analysis of letter-speech sound learning among dyslexic and normal readers vis-à-vis phonological awareness, rapid automatized naming, reading, and spelling. Participants were provided with 20 min of training aimed at learning eight new basic letter-speech sound correspondences, followed by a short assessment of mastery of the correspondences and word-reading ability in this unfamiliar script. Our results demonstrated that brief training is moderately successful in differentiating dyslexic readers from normal readers in their ability to learn letter-speech sound correspondences. The normal readers outperformed the dyslexic readers for accuracy and speed on a letter-speech sound matching task, as well as on a word-reading task containing familiar words written in the artificial orthography. Importantly, the new artificial script-related measures were related to phonological awareness and rapid automatized naming and made a unique contribution in predicting individual differences in reading and spelling ability. Our results are consistent with the view that a fundamental letter-speech sound learning deficit is a key factor in dyslexia.