Parallels between patterns of brain maturation and cognitive development have been observed repeatedly, but studies directly testing the relationships between improvements in specific cognitive functions and structural changes in the brain are lacking. Working memory development extends throughout childhood and adolescence and likely plays a central role for cognitive development in multiple domains and in several neurodevelopmental disorders. Neuroimaging, lesion, and electrophysiological studies indicate that working memory emerges from coordinated interactions of a distributed neural network in which fronto-parietal cortical regions are critical. In the current study, verbal working memory function, as indexed by performance on the Keep Track task, and volumes of brain regions were assessed at two time points in 79 healthy children and adolescents in the age range of 8–22 years. Longitudinal change in cortical and subcortical volumes was quantified by the use of Quantitative Anatomical Regional Change. Improvement in working memory was related to cortical volume reduction in bilateral prefrontal and posterior parietal regions and in regions around the central sulci. Importantly, these relationships were not explained by differences in gender, age, or intelligence level or change in intellectual abilities. Furthermore, the relationships did not interact with age and were not significantly different in children, young adolescents, and old adolescents. The results provide the first direct evidence that structural maturation of a fronto-parietal cortical network supports working memory development.