In sub-Saharan Africa, recent data about causes of adult death and care-seeking during illnesses are limited. This analysis examines adult deaths using verbal and social autopsy data from a nationally and provincially representative sample registration system in Mozambique. Causes of death among those 18 years and older were assigned using the InSilicoVA algorithm, and underlying social causes were examined using the pathway to survival model. Care-seeking was analyzed in different groups to determine if care was sought from formal providers (doctor, nurse/midwife, and trained community health worker) or other providers (traditional provider, family member, and pharmacist), using χ2 tests and multinomial regression models. Among the 4,040 adult deaths reported during 2019-2020, the major causes were HIV (17%), cancer (13%), injury (10%), cardiovascular diseases (9%), pneumonia (7%), tuberculosis (5%), and maternal causes (3%). Formal care-seeking was more likely among adults who had primary or higher level education (relative risk ratio [RRR]: 1.6, P < 0.001; RRR: 1.7, P < 0.01), were married (RRR: 1.3, P < 0.01), and had highest household wealth (RRR: 3.1, P < 0.001). Formal care-seeking was less likely among adults who were male (RRR: 0.7, P < 0.001), had social capital (RRR: 0.7, P < 0.05), or resided in the southern region (RRR: 0.4, P < 0.001). Information about adult causes of death is useful for formulating policy and for developing, monitoring, and evaluating programs to improve adult health in Mozambique. Care-seeking-related information helps identify barriers for seeking care from formal health providers while emphasizing the need for generating local resources and strengthening outreach health systems service delivery.