For Australians experiencing a suicide crisis, the emergency department (ED) is the recommended point of contact for intervention and to ensure personal safety. However, negative ED experiences can deter individuals from returning, thus impacting future suicide risk. In order to improve the ED environment for individuals in suicidal crisis, an in-depth understanding of this experience is needed. In-depth semi-structured interviews with 17 help seekers and 16 support persons were conducted. A grounded theory approach uncovered a core organising concept—all participants wanted a “a sustained, productive, constructive relationship with someone who can help” during the ED visit—which guided analysis. Thematic analysis resulted in two themes and four subthemes exploring the systemic and interpersonal aspects of the ED visit and the roadblocks and pathways to development of the relationship. Interpersonal factors included aspects of staff interaction and presence of a support person. Systemic factors related to aspects controlled by the physical space and internal policies and procedures and included aspects such as the chaotic environment, long waiting times, and access to staff. Overwhelmingly, there were more roadblocks than pathways reported by participants. Improving the ED environment, increasing staff training and encouraging the presence of support persons may help mitigate some of these roadblocks.