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Balanced medical and criminal justice approaches addressing determinants of alcohol and other drugs (AOD) use are central to achieving the United Nations Sustainable Development Goals 3 and 16. However, data on AOD use in resource-poor settings are characterised by relative paucity and anecdote. This study aimed to describe and analyse AOD use susceptibility and its determinants among school-attending adolescents in the capital Bissau, Guinea-Bissau. Survey data were collected through a locally adapted Planet Youth questionnaire in June 2017 across 16 schools in Bissau. The 2039-strong sample was selected through a multi-stage, random cluster process. Participants’ lifetime alcohol use was 27.3%, smoking 10.8%, and cannabis use 3.6%. In each instance, the ‘15 years and above’ age bracket was the most common initiation period, signifying increased instigation in later adolescence. Subsequent Varimax Principal Component Analysis (PCA) of 312 variables captured data-driven models of AOD use susceptibility, implying imitated, polydrug use among initiates. Linear regression analysis revealed drinking, group violence, male gender, school dismissal and relationship breakdown as explanatory variables. Overlapping predictive variables suggest singular interventions may pre-empt myriad antisocial behaviours. PCA offers alternatives to singular, potentially myopic quantifications of drug use. PCA facilitates the creation of context-sensitive composite variables, enabling the identification of related outcome behaviours relevant to studies’ sociocultural settings.