Background: The benefits of patient-focused pharmaceutical care in improving clinical outcomes and reducing health expenditure have been well documented. However, these services are not fully implemented in many developing countries like China, especially in the community setting at chain pharmacies. Methods: A cross-sectional questionnaire-based survey was conducted at nine chain pharmacies in eight provinces of China in late 2019 to assess the difference in attitude, perceived barriers, and expected facilitators of Chinese community pharmacists to deliver pharmaceutical care, as well as their willingness to develop the competencies based on age, education level, and seniority. A quantitative analysis of responses was undertaken by using nonparametric (Kruskal–Wallis) and chi-square tests (followed by Bonferroni post-hoc test). Results: A total of 1260 community pharmacists were enrolled in the survey. In total, 16.3% of participant pharmacists often felt that lack of ability had a negative impact on work especially when providing comprehensive medication guidance (39.0%); 44.4% were unsatisfied with academic degrees; 85.8% were “very willing” to improve ability of pharmaceutical care while only 46.9% and 38.4% regarded traditional practice and continuing education as of lots of help, respectively. Main barriers in capacity enhancement were linked to conflict with daily work (35.4%), conflict with family life (21.9%), and poor memories (15.3%). The most welcomed facilitators to enhance pharmaceutical care development included professional skills training (28.4%), self-study of online resources (20.3%), and adult education in universities (15.6%). Community pharmacists of different age, education level, and seniority held significantly different opinions on the above aspects (p < 0.05). Conclusion: Chinese community pharmacists showed a positive attitude towards capacity enhancement in pharmaceutical care. Specific efforts and reforms should be made to improve the professionalism and to remove barriers based on their age, different education level, and seniority.