The desire to die by suicide has been linked with interpersonal difficulties and impeded clinical outcomes. Despite the emphasis on the therapeutic relationship in clinical guidelines for working with suicidal clients, little is known about how suicidal clients' interpersonal difficulties manifest in clinical contexts. Additionally, there is limited understanding of the therapeutic relationship in single-session suicidal crisis contexts. Our aim was to examine the trajectory of the therapeutic bond in mediating clients' suicidal desire and outcome in single-session suicidal crisis intervention. Single-session online text-based crisis intervention sessions (N = 354; Mage = 29.43, SD = 9.15; 64.5% women) were coded for suicidal desire, therapeutic bond (each quarter), and outcome. We examined the proposed sequential mediating model (suicidal desire to early bond to bond change to outcome) using structural equation modeling. The proposed sequential mediation model fits the data well, χ2(11) = 22.030, p =.0241, root-mean-square error of approximation =.053, 90% CI [.019,.085], comparative fit index =.983, Tucker–Lewis index =.977, and was a better fit than several alternative models. Further, the indirect effect from suicidal desire to outcome through early bond and bond change was significant (b = −0.474, 99% CI [−0.782, −0.203]). Our findings indicate that therapeutic bonds were beneficial for clients with elevated suicidal desire—and—elevated suicidal desire was negatively associated with therapeutic bonds. These findings highlight the importance of training clinicians to navigate the unique challenges of developing therapeutic bonds with acutely suicidal clients. Public Significance Statement: Contemporary suicide theory has emphasized the interpersonal challenges that those with suicidal desire often experience. Our findings indicate that these challenges extend into the clinical context—greater suicidal desire was associated with poorer therapeutic bonds. Despite the difficulty in developing strong therapeutic relationships with suicidal clients, it is important that clinicians prioritize these relationships as we found a strong link between the therapeutic bond and suicidal clients' outcomes. [ABSTRACT FROM AUTHOR]