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Background: In recent years, virtual consultations have emerged as a crucial approach for continuity of chronic care provision, indicating a promising avenue for the future of smart healthcare systems. However, reversions to in-person care highlight persistent limitations, despite notable advantages of remote modalities. In parallel, recent developments in artificial intelligence (AI) indicate the potential to enhance remote chronic care, but user perceptions of such assistance and the corresponding human factors remain underexplored. Objective: This mixed methods study aims to better understand the virtual consultation experiences and attitudes toward AI-assisted tools in remote care among patients with noncommunicable chronic conditions and their healthcare professionals (HCPs). It conducts an in-depth examination of the associated human–computer interaction and usability elements of virtual consultations and of potential AI assistance. Methods: Public and Patient Involvement was integrated to run pilots and refine documentations. Semi-structured interviews with patients (n = 10), focus groups with HCPs (n = 15), and an online survey (n = 83) were conducted. Qualitative data was analysed through a reflexive thematic approach. The survey comprised the Telehealth Usability Questionnaire (TUQ) and bespoke items on user AI views, and the data was used to triangulate the qualitative findings. Nonparametric Kruskal–Wallis tests and ε2 effect sizes compared TUQ and AI views scores between current and former virtual consultation user groups. Results: Seven themes emerged from the qualitative data, which were supported by the quantitative findings. The statistical analyses resulted in a mean TUQ total score of 90.6 (SD = 15.0), which indicates high usability and user satisfaction; however, they failed to detect a difference between groups (p > 0.05; ε2 = 0.002–0.032). There was a clear preference for hybrid models, while a lack of empathy was identified during remote interactions. While a notable proportion of users indicated a literacy gap towards AI use in healthcare settings, they expressed cautious openness towards AI assistance, contingent upon transparency, human oversight, and data integrity; indicating a potential gap between competence to judge the technology and willingness to use it. Significant differences in views on AI assistance across groups failed to be detected (p > 0.05; ε2 = 0.005–0.065). Conclusions: Virtual consultations for chronic conditions are widely usable and acceptable, particularly through hybrid approaches. Addressing empathic engagement, holistic patient status, and transparent AI integration can enhance clinical quality and user experiences during remote interactions. However, the low statistical power and failure to detect a difference between groups (likely due to the small sample size) indicate the need for caution when interpreting the quantitative findings. There is also the implicit need to address potential AI literacy gap among users, indicating the need for robust safeguard measures. This study has also identified evidence-based assistive AI features that can potentially enhance virtual consultations. These insights can inform the co-design of evidence-based virtual care platforms, policies and supportive AI tools to sustain remote chronic care delivery.