Background: Breastfeeding is widely recognized as the optimal and natural method of feeding infants. However, there are obstacles that can limit exclusive breastfeeding practices during the first 6 months of an infant’s life. This study aimed to determine the prevalence of unsuccessful exclusive breastfeeding and its associated factors among mothers who work as healthcare providers at Universiti Sains Malaysia Hospital. Methods: A cross-sectional study was conducted among 295 medical doctors and staff nurses from June to December 2015. Simple random sampling was applied. The data were collected using a self-administered questionnaire and analyzed using IBM SPSS ver. 22.0 (IBM Corp., Armonk, NY, USA). Descriptive statistics and logistic regression analysis were performed. Results: The prevalence of unsuccessful exclusive breastfeeding among the study participants was 58.3%. Mothers who preferred formula milk (odds ratio [OR], 4.40; 95% confidence interval [CI], 1.45–13.31) delivered via lower segment cesarean section (OR, 2.31; 95% CI, 1.07–4.98) and produced inadequate breast milk (OR, 4.06; 95% CI, 2.40– 6.89) were significantly associated with unsuccessful exclusive breastfeeding. Conclusion The prevalence of unsuccessful exclusive breastfeeding among the study participants was high. Maternal characteristics such as preference towards formula milk, mode of delivery and adequacy of breast milk must be assessed to prevent unsuccessful exclusive breastfeeding among healthcare providers.