Introduction: The role of pharmacists in public health management is expected to grow into a key player in the continuing measures of managing the COVID-19 pandemic, especially in the community setting. However, their intention to provide essential public health services for combating the pandemic and the impact of their attitude and beliefs are largely unknown. This study aimed to investigate the intention-to-practice COVID-19-related responsibilities of pharmacists based on the theory of planned behavior (TPB), identify the key factors predicting their intention, and explore the usefulness of the TPB model in predicting such an intention. Methods: A cross-sectional, self-administered questionnaire was completed by pharmacists in Macao between May and August 2020. Quantitative responses regarding intention-to-practice COVID-19-related duties, and the four TPB variables [attitude (A), subjective norms (SN), perceived behavioral control (PBC), and past behavior (PB)] were measured. Cronbach's alpha and composite reliability were used to determine the reliability and validity of the tool. In addition to descriptive statistics, Pearson's correlation was used to determine the strengths of the association, and multiple linear regression was used to predict the association between the intention and the four key variables. Results: More than half of the pharmacists practicing in Macao completed the questionnaire (296/520) giving a response rate of 56.9%. Among them, 75% were 26–40 years old and 56% were female. The majority of the participants (91.9%) demonstrated a positive intention to contribute to the COVID-19 infection management (mean = 4.19 ± 0.51). The mean scores for A, SN, PBC, and PB were 4.06 ± 0.52, 3.71 ± 0.58, 3.76 ± 0.65, and 4.03 ± 0.54, respectively. A (β = 0.671), SN (β = 0.608), PBC (β = 0.563), and PB (β = 0.829) were all positively correlated with intention (all P < 0.001). It was found that 72.5% of the variance in the intention-to-practice COVID-19-related duties could be explained by the TPB model using the four key variables with A and PB being two possible predictors. Conclusion: Pharmacists showed favorable A, SN, PBC, and intention in participating in COVID-19 management in the community setting. Specific training, enhanced stakeholder communication, and improved pharmacy management are essential to increase the willingness of pharmacists to take part in the COVID-19 pandemic and other public health emergencies alike in the future.