Dental age estimation in the living and deceased is a fundamental aspect of forensic sciences, civil cases, medico-legal proceedings and clinical dentistry. Accordingly, this study aimed to validate the accuracy and reproducibility of the London Atlas in a select South African sample of KwaZulu-Natal. In this cross-sectional study, 760 digital panoramic radiographs (n = 760) aged between 5.00 and 23.99 years were retrospectively reviewed through consecutive sampling. Each radiograph was assessed and assigned a dental age in accordance with the London Atlas of Human Tooth Development and Eruption by AlQahtani et al. (2010). The London Atlas overestimated age with a mean difference of −0.85 to −1.26 years in the selected South African sample of KwaZulu-Natal. A statistically significant difference between the chronological and estimated dental ages was recorded. Furthermore, the South African Black and Indian males had a higher overestimation of age than their female counterparts, with a mean difference of 0.13 and 0.07 years, respectively. This overestimation was less in the South African Indian population in comparison to the SA Black population. This outcome resulted in the creation of the KZN population- and sex-specific charts and atlases for the two selected cohorts of KwaZulu-Natal. The KZN Atlases were found to be more accurate in the selected sample, with a mean absolute error of 0.57 years and no statistically significant differences between the chronological and estimated dental ages.