The urgent and reactive implementation of telemedicine during the pandemic does not represent a long-term, strategic, and proactive approach to optimizing this technology. The assumptions, perceptions, and experiences of the behavioral health providers using telemedicine can inform system-wide and institutional-level strategies to promote longitudinal maintenance of care delivery, which can reduce the use of high-cost care due to new symptom onset and symptom exacerbation related to service interruptions. We aim to identify the assumptions, perspectives, and experiences of behavioral health clinicians and providers using telemedicine to inform the development of an optimized, sustainable approach to telemedicine implementation. This qualitative study applies the domains of the Consolidated Framework for Implementation Research (CFIR) to structure data collection and analysis from behavioral health providers using telemedicine via an audiovisual connection in the New England region. In total, 12 providers across levels of care were recruited for a 60-minute interview, developed from the CFIR interview guide. Atlas Ti Qualitative Software (version 23; ATLAS.ti Scientific Software Development GmbH) was used to coordinate and facilitate coding among 3 reviewers. Deductive coding was provided from the CFIR interview guide, allowing for data to be categorized by domain and construct. Constructs were analyzed for descriptive themes and tabulated for response frequency. Uncoded data were reviewed and coded in vivo to explore variables contributing to participant perceptions of experience with telemedicine use. Descriptive themes, then analytical themes, were identified. Analytical themes and tabulated frequency of response data were summarized. Finally, a sentiment analysis was completed to derive tone and meaning from the data. Results are reported within the CFIR domains: intervention characteristic, outer setting, inner setting, characteristics of individuals, and process. The findings with ≥90% agreement include "best practice standards were not known"; "telemedicine was believed to be efficient and time-saving for the patient and provider, maximizing productivity and thus increasing access to care"; "telemedicine provided an additional option for patients to access services, promoting sustained continuity and timeliness of care"; "participants did not identify any clear goals related to telemedicine use"; "demonstrated positive affective responses to telemedicine use"; "expressed high efficacy with telemedicine utilization"; and "strong leadership support." These findings support the development of interstate compacts advancing licensure across state lines; payment parity across modalities of care to ensure the financial vitality of behavioral health services; improved dissemination of telehealth training and resources, and telehealth training in academic programs of the health professions; seamless, dynamic workflows to accommodate the changing needs of patient and care continuity; emergency response protocols; and community partnerships to provide private spaces needed for a therapeutic encounter. Future research exploring the patient's experience with telemedicine is needed for all stakeholders to be represented in developing a sustainable, integrated system.