Background: Oman’s healthcare system has rapidly transformed in recent years. A recent Report of Quality and Patient Safety has nevertheless highlighted decreasing levels of patient safety and quality culture among healthcare professionals. This indicates the need to assess the quality of care and patient safety from the perspectives of both patients and healthcare professionals. Objectives: This study aimed to examine (1) patients’ and healthcare professionals’ perspectives on overall quality of care and patient safety standards at two tertiary hospitals in Oman and (2) which demographic characteristics are related to the overall quality of care and patient safety. Methods: A cross-sectional study design was employed. Data were collected by two items: overall quality of care and patient safety, incorporated in the Revised Humane Caring Scale, and Healthcare Professional Core Competency Instrument. Questionnaires were distributed to (1) patients (n = 600) and (2) healthcare professionals (nurses and physicians) (n = 246) in three departments (medical, surgical and obstetrics and gynaecology) at two tertiary hospitals in Oman towards the end of 2018 and the beginning of 2019. Descriptive statistics and binary logistic regression were used for data analysis. Results: A total of 367 patients and 140 healthcare professionals completed the questionnaires, representing response rates of 61.2% and 56.9%, respectively. Overall, quality of care and patient safety were perceived as high, with the healthcare professionals rating quality of care (M = 4.36; SD = 0.720) and patient safety (M = 4.39; SD = 0.675) slightly higher than the patients did (M = 4.23; SD = 0.706), (M = 4.22; SD = 0.709). The findings indicated an association between hospital variables and overall quality of care (OR = 0.095; 95% CI = 0.016–0.551; p = 0.009) and patient safety (OR = 0.153; 95% CI = 0.027–0.854; p = 0.032) among healthcare professionals. Additionally, an association between the admission/work area and participants’ perspectives on the quality of care (patients, OR = 0.257; 95% CI = 0.072–0.916; p = 0.036; professionals, OR = 0.093; 95% CI = 0.009–0.959; p = 0.046) was found. Conclusions: The perspectives of both patients and healthcare professionals showed that they viewed both quality of care and patient safety as excellent, with slight differences, indicating a high level of patient satisfaction and competent healthcare delivery professionals. Such perspectives can provide meaningful and complementary insights on improving the overall standards of healthcare delivery systems.