This study examines the association between nurses’ perception of caring and attitudes toward caring for dying patients in end-of-life care units. We used a descriptive cross-sectional design with convenience sampling. Data were collected from May to June 2021 through self-reported questionnaires from 303 Spanish nurses (mean age = 48 years, 78.9% female). Participants completed the Caring Dimension Inventory (CDI-25) and the Frommelt Attitudes Toward Care of the Dying scale. Demographic and training information were collected. Data were analyzed using Stata 16.0. Attitudes toward Care of the Dying Patient were significantly higher in nurses with palliative care training (β = 2.829, p = 0.018) and those who scored higher on the psychosocial (β = 0.789, p = 0.0001) and technical dimensions (β = 0.487, p = 0.011) of the CDI-25. Multivariate analysis identified the psychosocial dimension of the CDI-25 scale (β = 0.783, p = 0.0001) and palliative care training (β = 2.686, p = 0.017) as the only significant variables associated with Attitudes toward Care of the Dying Patient. Overall, nurses exhibited a positive attitude toward caring for dying patients. Our results could potentially help nursing directors identify those with the necessary qualities and training for optimal end-of-life care and to further plan training courses to provide optimal care in end-of-life situations.