Background The COVID-19 pandemic has resulted in unprecedented uptake of telepsychology services; however, clinicians have mixed attitudes toward virtual technologies. Objective This study (1) explored clinicians’ experiences of and intentions to use video, telephone, and in-person services, and (2) tested the utility of the unified theory of acceptance and use of technology (UTAUT) to predict clinicians’ intentions to offer telepsychology after the COVID-19 pandemic. Methods Clinician satisfaction and therapeutic alliance were compared across in-person, video, and telephone services, while technology attitudes and intention to use after the pandemic were compared across video and telephone services among 118 addiction and mental health clinicians during the COVID-19 pandemic. Results Clinicians reported more positive experiences with in-person services than both virtual technologies; further, clinicians reported greater positive experiences, attitudes, and intentions to use video services than telephone services across measures. Based on the UTAUT, performance expectancy positively predicted concurrent intentions to use video services (β=0.46; P<.001) and telephone services (β=0.35; P<.001) after the pandemic. Social influence (β=0.24; P=.004) and facilitating conditions (β=0.19; P=.03) additionally predicted the intention to use telephone services. Conclusions Clinicians rated in-person services more positively than virtual technologies, with video services perceived more positively than telephone services. Performance expectancy was the primary facilitator of the uptake of both virtual modalities.