Introduction Sibling designs in assessing familial aggregation and risk prediction of dental caries have been largely unutilized. This large-scale investigation evaluated the robustness of parental socioeconomic position (SEP) as a cardinal determinant of caries experience by appraising it at the family level. Moreover, sibling-specific aggregation of caries within families and the discriminant ability of sibling caries in predicting co-sibling caries was ascertained. Methods A nationwide, register-based cross-sectional study was conducted on Danish adolescent siblings (n = 23,847 sibling pairs; index siblings/probands: all 15-year-olds in 2003; co-siblings: biological siblings born to the same mother within ± 3 years). Clinical (caries) data for each study subject were acquired from the national dental database (Sundhedsstyrelsens Centrale Odontologiske Register [SCOR]). Data on social variables, namely, parental SEP (parental education, income, and occupation), ethnicity, age/birth order, gender, and household type, were compiled from administrative registers at Statistics Denmark (e.g., the Danish population, education, labor market affiliation, and income and transfer payments registers). The social gradient in the magnitude of caries experience among the index- and co-siblings was estimated using negative binomial regression and generalized estimating equations taking into account family level clustering. Familial aggregation of caries was ascertained using probandwise concordance rates and adjusted pairwise odds ratios (PORs) from alternating logistic regressions. In order to determine the discriminant ability of proband caries and that of the other study covariates to effectively predict the absence or presence of caries in a sibling, a classification and regression tree (CART) analysis was undertaken. The predictive power of the CART models was evaluated using the area under the Receiver Operating Characteristic curve (AUROC) statistic. Results The prevalence of dental caries experience in the overall study population was 73.6% (index siblings 74.3%, co-siblings 72.9%). Conspicuous social patterning of caries was observed in both the index- and co-sibling populations even after adjustment for all study covariates. Significant sibling-specific familial aggregation of caries was observed, which varied in a stepwise graded fashion across the social hierarchy. Overall, 70.6% of sibling pairs were concordant in terms of their caries experience (caries 58.9%, caries-free 11.7%). Co-siblings of affected probands had 3.9 times (95% CI: 3.65–4.18) higher (adjusted) odds of having caries compared to those with caries-free siblings. This sibling similarity was further amplified in those with relative socioeconomic disadvantage (e.g., the adjusted PORs varied from 3.39 [95% CI: 3.04–3.77] in the highest to 5.47 [95% CI: 4.36–6.86] in the lowest parental education category). AUROCs from the CART models ranged from 0.7–0.82, indicating useful to excellent overall predictive power of the models. These models revealed sibling (proband) caries experience to be the single-most important risk predictor of caries in individuals (co-siblings), with the results indicating that caries could be expected in ≥ 84% of siblings of adolescents with 3 or more caries-affected tooth surfaces. Conclusions Graded clustering patterns of caries and socioeconomic disadvantage are encapsulated within families in Denmark, contributing to the engendering of health inequalities in society. With sibling caries being such a pertinent marker of increased caries risk, caries in a sibling should elicit preventive family-based approaches targeting co-siblings, particularly in socially disadvantaged households. Since caries shares common risk factors with other non-communicable diseases and conditions (such as diabetes and obesity), such policy constructs could reduce not only caries experience but also wider health inequalities in society.