Highlights • We nested a measles and rubella serological survey in a vaccination coverage survey. • Measles and rubella immunity was significantly higher than expected by vaccination. • Study revealed immunity gap in young adults and risk of congenital rubella syndrome. • Adding serology to a survey leveraged resources and provided complementary information. Abstract Background Serological surveys can potentially complement vaccine coverage surveys, such as post-vaccination campaign coverage evaluation surveys (PCES), by providing direct information on population immunity within and outside the target age range of the mass vaccination campaign. We estimate age-specific population immunity to measles and rubella viruses in Southern Province, Zambia, and assess the value of adding serological data to vaccination coverage estimates by nesting a serological survey within a PCES. Methods Dried blood spots (DBS) from fingerprick blood were collected from all individuals ages nine months or older in households participating in the PCES and tested for measles and rubella virus-specific immunoglobulin G (IgG) by enzyme immunoassay (Siemens Enzygnost, Marburg, Germany). Results Overall seroprevalence was 95.5% (95% CI: 92.8, 97.2) for measles virus-specific IgG and 97.7% (95% CI: 96.0, 98.7) for rubella virus-specific IgG. Rubella seroprevalence was 98.4% (95% CI: 95.9, 99.4) among children eligible for the MR vaccination campaign, significantly higher than the reported measles-rubella (MR) vaccination campaign coverage of 89.8% (p = 0.003), and higher than the 91.3% rubella seroprevalence for adolescents and adults 16–30 years of age (p = 0.049). Conclusion Seroprevalence to measles and rubella viruses in children younger than 16 years of age was significantly higher than expected from vaccination coverage estimates, likely reflecting exposure to wild-type viruses and underreporting of vaccination. The serosurvey revealed rubella immunity gaps among women 16–30 years of age, precisely the age group in which protection from rubella is most important to prevent congenital rubella syndrome. Nesting serological surveys within existing surveys can leverage resources and infrastructure while providing complementary information important to immunization programs. [ABSTRACT FROM AUTHOR]