Background: Assessing the elements of nursing practice environments is crucial, as investing in their improvement will enhance outcomes for nurses, patients, and organizations. Moreover, comparing practice environments from different countries improves the definition of cross-cutting guidelines that can be applied in various contexts. Thus, this study aims to evaluate nursing practice environments in hospitals in Portugal and Brazil. Methods: A multicenter and cross-sectional study was conducted in eight Portuguese and eight Brazilian hospitals. Five hundred eighty-two nurses completed a survey regarding their sociodemographic and professional attributes, as well as the Scale for the Environments Evaluation of Professional Nursing Practice. The data were subjected to comparative analyses between the two countries. We adhered to ethical requirements in both participating countries. Results: In Brazil, the Structure, Process, and Outcome components were considered favorable to the quality of care and well-being of nurses. In Portugal, nurses considered the Structure and Outcome components favorable and the Process component very favorable. Statistically significant differences were found between the two countries in several dimensions of the three subscales. The Structure and Outcome components scored significantly better in hospitals in Brazil, and the Process component scored better in Portuguese hospitals. Conclusions: These conclusions underscore the urgent need for investment in continuous training and a culture of evaluation that promotes continuous improvement. Additionally, promoting the involvement and participation of nurses could simultaneously contribute to the development of more sustainable health systems.