Research indicates the primary difference between strong and weak readers is their phonemic awareness skills. However, there is no consensus regarding which specific components of phonemic awareness contribute most robustly to reading comprehension. In this study, the relationship among sound blending, sound segmentation, and reading comprehension is investigated. A total of 84 African American and two multiethnic 1st- through 4th-grade students attending an inner-city charter school completed measures of sound blending, sound segmentation, and reading comprehension. Statistically significant relationships were found between blending and segmenting skills and blending and reading comprehension. Results from structural equation modeling reveal a moderate to large effect size between sound blending and reading comprehension and a relatively small effect size between sound segmenting and reading comprehension. The results indicate sound blending skills account for more variance in the prediction of reading comprehension than segmenting skills with this unique research population. Implications for early instruction and intervention are discussed.