Global progress toward universal health coverage (UHC) has varied widely across low- and middle-income countries (LMICs) in recent years. To better understand these differences, we used an analytical framework to compare individual health system components, or substructures, across selected LMICs, identifying institutional and policy mechanisms that shape UHC performance. Our case study comparison includes 12 countries spanning high and low UHC performance, as indicated by World Bank and World Health Organization (WHO) indicators for service coverage and financial risk protection as well as considerations of equity concerns not captured by these metrics. We highlight that stronger performance is associated with unified risk pooling, strategic purchasing, robust primary care–based integrated delivery, a systemic approach toward public/private service delivery, strategic investments in health infrastructure and workforce, and accountable governance. Future analyses and reviews using this comparative case study method with a structured analytical framework would be helpful in further advancing our understanding of the drivers of UHC progress and guiding policy reform.