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Introduction Deliberate self-poisoning is a leading method of self-harm among adolescents globally. This study aimed to identify psychosocial, familial and contextual risk factors associated with deliberate self-poisoning among Sri Lankan adolescents.Methods A multicentre prospective case–control study was conducted across selected tertiary care hospitals in Sri Lanka over a 2-year period. Adolescents aged 10–17 years admitted with deliberate poisoning were recruited as cases. Age- and sex-matched controls were recruited from the same study settings. Structured interviews were conducted using a pretested tool assessing sociodemographic, psychological, family and school-related factors. Conditional logistic regression was used to estimate adjusted ORs (AORs) and 95% CIs.Results A total of 326 case–control pairs (n=652) were included. The majority of cases were female (74.5%) and aged 15–17 years. The most frequently ingested agents were paracetamol (45.1%) and oleander (10.7%). In multivariable analysis, personal history of psychiatric illness (AOR 2.76, 95% CI 1.92 to 5.41), previous self-injury (AOR 4.17, 95% CI 1.92 to 10.77), previous deliberate poisoning (AOR 4.02, 95% CI 2.86 to 5.19), non-heterosexual orientation (AOR 26.9, 95% CI 12.18 to 75.45), school dropout (AOR 4.01, 95% CI 2.06 to 6.57), home violence (AOR 8.93, 95% CI 3.27 to 26.47) and feeling depressed (AOR 2.08, 95% CI 1.49 to 3.20) were independently associated with deliberate poisoning.Conclusion Deliberate self-poisoning among Sri Lankan adolescents is strongly associated with psychiatric comorbidity, family adversity, sexual identity-related distress and school disengagement. These findings highlight the urgent need for integrated, adolescent-friendly mental health services, school-based screening and psychosocial support mechanisms.