Reading is a complex process involving recruitment and coordination of a distributed network of brain regions. The present study sought to establish a methodologically sound evidentiary base relating specific reading and phonological skills to neuro-metabolic concentration. Single voxel proton magnetic resonance spectroscopy was performed to measure metabolite concentration in a left hemisphere region around the angular gyrus for 31 young adults with a range of reading and phonological abilities. Correlation data demonstrated a significant negative association between phonological decoding and normalized choline concentration and as well as a trend toward a significant negative association between sight word reading and normalized choline concentration, indicating that lower scores on these measures are associated with higher concentrations of choline. Regression analyses indicated that choline concentration accounted for a unique proportion of variance in the phonological decoding measure after accounting for age, cognitive ability and sight word reading skill. This pattern of results suggests some specificity for the negative relationship between choline concentration and phonological decoding. To our knowledge, this is the first study to provide evidence that choline concentration in the angular region may be related to phonological skills independently of other reading skills, general cognitive ability, and age. These results may have important implications for the study and treatment of reading disability, a disorder which has been related to deficits in phonological decoding and abnormalities in the angular gyrus.