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<b></b> <i>Background:</i> Globally over 720,000 deaths yearly are due to suicide, approximately 20% due to pesticide self-poisoning. Poor school-connectedness has been shown to be associated with increased risk of suicidal thoughts and behaviors in high-income countries, while good school-connectedness is protective of suicidality. This study investigated associations between poor school-connectedness and self-poisoning in a low- and middle-income country. <i>Methods:</i> We used data collected in a hospital-based case-control study in rural Sri Lanka. Cases (<i>n</i> = 298) were adults admitted due to self-poisoning, and controls (<i>n</i> = 596) frequency matched on age and sex. Structured interviews assessed school-connectedness using four questions, and data on confounders (ethnicity, parental migration, child adversity, and parental education) were also collected. Associations were quantified using logistic regression. <i>Results:</i> Individuals with poorer relationships with other students (<i>OR</i> = 1.90, 95% CI 1.22, -2.95) and lower levels of school enjoyment (<i>OR</i> = 1.34, 95% CI 0.94, -1.92) were more likely to present for self-poisoning in adulthood. They were also more likely to report poor relationships with teachers, but this relationship was not as strong (<i>OR</i> = 1.30, 95% CI 0.90, -1.88). <i>Limitations</i>: The questionnaire used is not validated in this setting. Additionally, this is a retrospective study using a hospital sample, which may be impacted by recall bias and/or excluding individuals who did not seek hospital treatment. <i>Conclusions:</i> Interventions to improve school-connectedness in Sri Lanka, with a particular focus on relationships between students, may reduce self-poisoning in adulthood. Further research is needed to explore how to achieve this, and to understand the reasons for association between school-connectedness and self-poisoning.