While a growing number of studies have highlighted the potential of virtual reality (VR) to improve athletes’ skills, no research has yet focused on acceptance of a VR head-mounted display (VR-HMD) designed to increase sport performance. However, even if technological devices could potentially lead to performance improvement, athletes may not always accept them. To investigate this issue, the Technology Acceptance Model (TAM) examines if perceived usefulness, perceived ease of use, perceived enjoyment, and subjective norms (i.e., social influence) are positive predictors of intention to use a specific technology. The aims of the present study were to test with competitive athletes the validity of the TAM before a first use of a VR-HMD intended to enhance sport performance and to examine to what extent the level of practice and the type of sport practiced have an influence on the previous variables of the TAM. The study sample comprised 1162 French athletes (472 women, 690 men, Mage = 24.50 ± 8.51 years) who usually practiced a sport in competition (from recreational to international level). After reading a short text presenting the VR-HMD and its interests for sport performance, the participants filled out an online questionnaire assessing their acceptance of this technological device before a first use. The results of the structural equation modeling analysis revealed that perceived usefulness, perceived ease of use, perceived enjoyment, and subjective norms were positive predictors of intention to use this VR-HMD, validating the suitability of the TAM for investigating the acceptance by athletes of a VR-HMD designed to increase their sport performance. The results also showed that athletes of all sport levels (a) had a significant intention to use VR, (b) found it quite useful (except for recreational athletes), quite easy to use, and quite pleasant to use, even if their entourage would not encourage them to use it (except for international athletes), and (c) found the VR-HMD easy and pleasant to use whatever the sport practiced. Notably some athletes (e.g., triathletes, swimmers, cyclists) did not find the VR-HMD significantly useful and did not have significant intention to use it to increase their performance. Identifying acceptance by athletes of such a device may increase the likelihood that it will be used by athletes of different levels and from different sports, so that they can benefit from all its advantages related to the improvement of their sport performance. Needs-based targeted interventions may also be conducted toward athletes who might be reluctant to integrate this type of device into their training.