Background: Health literacy is an important determinant of health, but national health literacy levels are known for only some European countries. This study aims to examine to what extent national health literacy levels can be estimated based on publicly available census data. Method: Multivariate models were used to predict two types of health literacy on population level. Predictors were selected based on literature, the European Health Literacy Survey (HLS-EU) and the Adult Literacy and Life Skills Survey (ALL). The HLS-EU provides insight into self-assessed health literacy and the ALL into the performance of individuals on health literacy tasks (performance-based health literacy). Dutch HLS-EU and ALL data were used to construct prediction models based on 2/3 of this data, which were validated in the remaining 1/3 of the data and (in case of self-assessed health literacy) in data from seven other European countries. Results: Education is a significant predictor of perceived and performance-based health literacy. Age and working status are significant predictors of performance-based health literacy, whereas gender and income are significant predictors of self-assessed health literacy. Both typologies of health literacy can satisfactorily be predicted within samples of the Dutch population. The accuracy of estimated self-assessed health literacy varied between the seven other European countries. Conclusion: Prediction models based on publicly available census data can be used for estimating self-assessed and performance-based health literacy on population level. Observed health literacy levels or better prediction models are required when one is interested in ranking European countries.