This study presents new data sets on long-run enrollment ratios, educational attainment, and human capital stock measures for numerous countries. We construct a complete data set of historical enrollment ratios, subdivided by education level and gender, for 111 countries from 1820 to 1945 (at five-year intervals) by using newly compiled census observations and information on the year of establishment of the oldest school in individual countries. Then, by utilizing these enrollment ratios, as well as available census data from 1945 onward on different age groups’ educational attainment, we construct a data set of estimated educational attainment, disaggregated by gender and age group, and aggregate human capital stock that spans from 1870 to 2010. The data show that over the past two centuries, there has been remarkable growth in average educational attainment and human capital stock as well as a narrowing of the gap in average educational attainment between nations.