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Background: Home care workers (HCWs) are increasingly caring for patients with heart failure (HF). Previous studies have shown that they contribute to HF patients' care, but how their preparedness and their relationship with patients (mutuality) influence caregiving is unknown, as well as the role of HCWs' self-efficacy. Objective: Guided by the Situation-Specific Theory of Caregiver Contribution to HF Self-Care, we investigated the influence of HCWs' preparedness and mutuality on HCWs' contribution to HF self-care and the mediating effect of HCWs' self-efficacy in the process. Methods: We conducted a cross-sectional survey of HCWs who cared for patients with HF. The survey included the Caregiver Preparedness Scale, Mutuality Scale, Caregiver Contribution to Self-Care of HF Index, and Caregiver Self-Efficacy in Contributing to Self-Care Scale. We performed structural equation modeling and a mediation analysis. Results: A total of 317 HCWs employed by 22 unique home care agencies across New York, NY, completed the survey. They had a median age of 50 years, 94% were women, and 44% were non-Hispanic Black. Results demonstrated that mutuality had a direct influence on HCW contribution to self-care and preparedness influenced their contribution to self-care, but only through the mediation of self-efficacy. Conclusion: Home care workers' preparedness, mutuality, and self-efficacy have important roles in influencing their contribution to HF self-care. As a workforce increasingly involved in the care of patients with HF, knowing the mechanisms underpinning HCWs' contribution to self-care may illuminate future interventions aimed at improving their contributions and HF patient outcomes.