Despite accelerating interest in the impact of the internet on suicidal behaviour, empirical work has not captured detailed narratives from those who engaged in suicide-related internet use. This study explored the suicide-related online behaviour of two contrasting samples of distressed users, focusing on their purpose, methods and the main content viewed. In-depth interviews were conducted in the UK between 2014-2016 with i) young people in the community; and ii) self-harm patients presenting to hospital emergency departments. Data were analysed using methods of constant comparison. Suicide-related internet use varied according to the severity of suicidal feelings. In the young people sample, where severity was lower, use was characterised by disorganised browsing without clear purpose. A range of content was 'stumbled upon' including information about suicide methods. They also pursued opportunities to interact with others and explore online help. Self-harm patients were a higher severity group with a history of suicidal behaviour. Their use was purposeful and strategic, focused around 'researching' suicide methods to maximise effectiveness. They made specific choices about content viewed; many consulting factual content in preference to user generated accounts, while help content and communication was avoided. Findings indicate further action is necessary to improve online safety. Also, novel online help approaches are needed to engage individuals experiencing suicidal crisis. Awareness of the nature of suicide-related internet use and how this may reflect the status of an individual's suicidal thinking could be beneficial to clinicians to promote safety and indicate risk.