The Chilean government is implementing strategies to improve hospital care but has not addressed the potential contributions of the nursing workforce and the work environment to achieve quality outcomes. Extensive international evidence demonstrates that work environments are associated with nurse job outcomes and patient outcomes, including care experiences. The aim of this study was to evaluate the quality of the nurse work environment in a nationally representative sample of hospitals in Chile and to analyze associations of the work environment with nurse job outcomes and patient care experiences. Utilizing a cross-sectional design, surveys were collected from 1,632 registered nurses and 2,017 patients on medical-surgical units in 40 adult general hospitals. Nurse informants and patients surveyed averaged 40.8 and 50.4 per hospital, respectively. The work environment was measured through the Practice Environment Scale of the Nursing Work Index, aggregated from survey responses to the hospital level. Nurse job outcomes included burnout, job dissatisfaction, and intent to leave. Patient care experience measures included hospital rating, likelihood of recommending the hospital, satisfaction with nursing care, and satisfaction with pain control. Adjusted logistic regression models were used to test associations of the work environment with outcomes. Nurses in hospitals with poor work environments, as compared to good, had significantly higher odds of experiencing burnout (OR: 1.50, 95% CI: 1.13-1.99, p < 0.005), job dissatisfaction (OR: 1.84, 95% CI: 1.28-2.64, p < 0.001), and intent to leave (OR: 1.45, 95% CI: 1.05-2.01, p < 0.024). Patients in hospitals with poor work environments, as compared to good, had lower odds of all care experience outcomes, but results were only significant for satisfaction with nursing care (OR: 0.56, 95% CI: 0.37-0.86, p < 0.008). Patients in hospitals with mixed work environments, as compared to good, had significantly lower odds of being satisfied with pain control (OR: 0.62, 95% CI: 0.48-0.82, p < 0.001). The work environment in Chilean hospitals is significantly associated with nurse job outcomes and patient care experiences related to nursing, including communication and pain control. Improving hospital work environments holds promise for improving nurse outcomes and retention as well as patient care experiences.