Background: The suicide rate in Guyana has consistently ranked in the top ten globally, yet there is only limited literature related to the context in which these suicides occur. This study aims to better understand the psychosocial circumstances and characteristics of suicides in Guyana. Methods: This case series study utilised a qualitative psychological autopsy method. One to three informants per deceased person (N = 31) were interviewed regarding the lives of 20 Guyanese who died by suicide (14 M, 6 F, aged 10–74 years). Interpretative Phenomenological Analysis was utilised for the data. Findings: Four superordinate themes were identified: Interpersonal Conflict, Trauma, Health, and Unknown Reasons. Interpersonal conflict included subordinate themes of Domestic Abuse, Marital Separation, and Financial Disputes. Health included subordinate themes of Physical Health and Mental Health. Pesticide poisoning was the method used by Guyanese people whose suicide was triggered primarily by interpersonal conflict. Interpretation: The findings illustrate the complexities of suicide in Guyana and the importance of adopting a biopsychosocial perspective to suicide prevention. Suicide prevention should include mental health and suicide literacy training of medical professionals. It is recommended that the importation of highly toxic pesticides be restricted, and that less toxic substitutes be promoted. Convenience sampling, recall bias, and limited informants are limitations of this study. Future research should focus on suicidal behaviour using larger sample sizes. Funding: This research was supported by an Australian Government Research Training Program Scholarship through Griffith University Australia.