Background The COVID-19 pandemic caused a surge in the use of telehealth platforms. Psychologists have shifted from face-to-face sessions to videoconference sessions. Therefore, essential information that is easily obtainable via in-person sessions may be missing. Consequently, therapeutic work could be compromised. Objective This study aimed to explore the videoconference psychotherapy (VCP) experiences of psychologists around the world. Furthermore, we aimed to identify technological features that may enhance psychologists’ therapeutic work through augmented VCP. Methods In total, 17 psychologists across the world (n=7, 41% from Australia; n=1, 6% from England; n=5, 29% from Italy; n=1, 6% from Mexico; n=1, 6% from Spain; and n=2, 12% from the United States) were interviewed. We used thematic analysis to examine the data collected from a sample of 17 psychologists. We applied the Chaos Theory to interpret the system dynamics and collected details about the challenges posed by VCP. For collecting further information about the technology and processes involved, we relied on the Input-Process-Output (IPO) model. Results The analysis resulted in the generation of 9 themes (input themes: psychologists’ attitude, trust-reinforcing features, reducing cognitive load, enhancing emotional communication, and engaging features between psychologists and patients; process themes: building and reinforcing trust, decreasing cognitive load, enhancing emotional communication, and increasing psychologist-patient engagement) and 19 subthemes. Psychologists found new strategies to deal with VCP limitations but also reported the need for more technical control to facilitate therapeutic processes. The suggested technologies (eye contact functionality, emergency call functionality, screen control functionality, interactive interface with other apps and software, and zooming in and out functionality) could enhance the presence and dynamic nature of the therapeutic relationship. Conclusions Psychologists expressed a desire for enhanced control of VCP sessions. Psychologists reported a decreased sense of control within the therapeutic relationship owing to the influence of the VCP system. Great control of the VCP system could better approximate the critical elements of in-person psychotherapy (eg, observation of body language). To facilitate improved control, psychologists would like technology to implement features such as improved eye contact, better screen control, emergency call functionality, ability to zoom in and out, and an interactive interface to communicate with other apps. These results contribute to the general perception of the computer as an actual part of the VCP process. Thus, the computer plays a key role in the communication, rather than remaining as a technical medium. By adopting the IPO model in the VCP environment (VCP-IPO model), the relationship experience may help psychologists have more control in their VCP sessions.