While there has been great success in increasing the coverage of new childhood vaccines globally, expanding routine immunization to reliably reach all children and communities has proven more challenging in many low- and middle-income countries. Achieving this requires vaccination strategies and interventions that identify and target those unvaccinated, guided by the most current and detailed data regarding their size and spatial distribution. Through the integration and harmonisation of a range of geospatial data sets, including population, vaccination coverage, travel-time, settlement type, and conflict locations. We estimated the numbers of children un- or under-vaccinated for measles and diphtheria-tetanus-pertussis, within remote-rural, urban, and conflict-affected locations. We explored how these numbers vary both nationally and sub-nationally, and assessed what proportions of children these categories captured, for 99 lower- and middle-income countries, for which data was available. We found that substantial heterogeneities exist both between and within countries. Of the total 14,030,486 children unvaccinated for DTP1, over 11% (1,656,757) of un- or under-vaccinated children were in remote-rural areas, more than 28% (2,849,671 and 1,129,915) in urban and peri-urban areas, and up to 60% in other settings, with nearly 40% found to be within 1-hour of the nearest town or city (though outside of urban/peri-urban areas). Of the total number of those unvaccinated, we estimated between 6% and 15% (826,976 to 2,068,785) to be in conflict-affected locations, based on either broad or narrow definitions of conflict. Our estimates provide insights into the inequalities in vaccination coverage, with the distributions of those unvaccinated varying significantly by country, region, and district. We demonstrate the need for further inquiry and characterisation of those unvaccinated, the thresholds used to define these, and for more country-specific and targeted approaches to defining such populations in the strategies and interventions used to reach them.