Background An evaluation of patient satisfaction with service provided in the health care system has been globally recognized as the measure of health care service quality. However, there is a lack of research findings that indicate patient satisfaction with newly implemented patient-oriented pharmaceutical care (PC) service provided by clinical pharmacists in Ethiopia. Therefore, the current study is aimed to determine the level of patient satisfaction and associated factors with PC service provided by clinical pharmacists in the Southwestern Ethiopia. Methodology A facility-based cross-sectional study design was employed among patients admitted to Medical wards in Jimma University Medical Center (JUMC) (n=219) from May to June 2021. The pretested interviewer-administered questionnaire containing structured questions on a 5-point Likert scale was appropriately completed and returned for statistical analysis. For the analysis of data, Statistical Package for Social Sciences (SPSS) was used. The associations between status of patient satisfaction and predictors were determined at 5% (p<0.05) level of significance by employing multivariate logistic regression. Results The current study revealed that more than half (56%) of the respondents were satisfied with clinical pharmacy service. From 30% of drug therapy problems (DTPs) reported, non-adherence was the most prevalent (11.4%), while the dose being too low and adverse effects (0.9%) were the least reported. Moreover, the assignment particular clinical pharmacist (AOR: 2.091, 95% CI: 1.028, 4.255), previous admission (AOR: 0.459, 95% CI: 0.244, 0.86), number of medications taken per day (AOR: 1.929, 95% CI: 1.996, 3.739) and length of hospital stay (AOR: 2.236, 95% CI: 1.124, 4.446) were significantly associated with patient satisfaction. Conclusion The present study revealed that patient satisfaction towards PC was low. Lack of specific clinical pharmacist assignment, previous history of admission, number of medications taken per day and length of hospital stay are revealed as the major factors affecting the level of satisfaction. In addition, current findings implicate that clinical pharmacist collaboration with a multidisciplinary team is essential to increase patient satisfaction.