Healthcare professionals constantly face situations that reflect ecosystems’ degradation. These can negatively affect their mental health. Research suggests that hope and resilience can play an important role in this scenario, since they are related to/predict mental health in highly heterogeneous samples (considering geography, age, profession, health, etc.). In this context, the aims of the present study are the following: to characterize and explore the relationship between hope, resilient coping and mental health in Portuguese healthcare professionals. Using Google Forms, 276 healthcare professionals answered the GHQ-28, the (adult) Trait Hope Scale, and the Brief Resilient Coping Scale (retrospective, analytical observational, cross-sectional, descriptive and correlational research design). The minimum and maximum possible scores were reached, with the exception of the maximum score of GHQ-28-Total. Regarding Hope, 19.6% scored below the midpoint (M = 43.46, SD = 11.97); 29.3% revealed low resilience (M = 14.93, SD = 4.05); and the average of four of the five Mental Health scores (exception: Severe depression) indicates the probability of a psychiatric case. Hope correlated with Social dysfunction and GHQ-28-Total; resilient coping proved to be a (weak) predictor of four of the five GHQ-28 indicators (exception: Severe depression). The results support the need to promote the sample’s mental health, hope and resilient coping. They also suggest that stimulating resilient coping may contribute to improving healthcare professionals’ mental health. Prior research (e.g., on therapies to enhance hope, resilience and, thus, mental health), to which the current study contributes, supports optimism towards the necessary internal sustainability transition.