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Background Illicit drug use is a well-established risk factor for morbidity and mortality. However, few studies have examined the impact of different drug use patterns on mortality among polysubstance using populations. This study aimed to identify drug-specific patterns of mortality among a cohort of polysubstance using persons who inject drugs (PWIDs). Methods PWIDs in Vancouver, Canada were prospectively followed between May 1996 and December 2011. Participants were linked to the provincial vital statistics database to ascertain mortality rates and causes of death. We used multivariate Cox proportional hazards regression to investigate the relationships between drug use patterns (daily alcohol use, heroin injection and non-injection use, cocaine injection, amphetamine injection and non-injection use, crack smoking and speedball injecting) and time to all-cause mortality. Results 2330 individuals were followed for a median of 61 months (inter-quartile range: 33 – 112). In total, 466 (19.1%) individuals died for an incidence density of 3.1 (95% confidence interval [CI]: 2.8 – 3.4) deaths per 100 person-years. In multivariate analyses, after adjusting for HIV infection and other potential confounders, only daily cocaine injection remained independently associated with all-cause mortality (adjusted hazard ratio [AHR] = 1.36, 95% CI: 1.06 – 1.76). Conclusions Although heroin injecting is traditionally viewed as carrying the highest risk of mortality, in this setting, only daily cocaine injecting was associated with all-cause mortality. These findings highlight the urgent need to identify novel treatments and harm reduction strategies for cocaine injectors.