This study examined the level of use and the level of self-efficacy use of mLearning devices for faculty at one university. The study also examined the relationship between use and self-efficacy levels, and the challenges faced by faculty members concerning the use of mLearning devices for professional activities. A mixed-methods model was used to complete the study. A 17-item self-report survey was developed by the researcher to determine the frequency of use, and the self-efficacy level of faculty concerning professional activities. An interview protocol was used to collect additional information from selected respondents. Findings indicated statistically significant differences in mean level of use scores for each of the 17 professional activities, but no overall significant differences in mean level of use scores based on selected demographic characteristics. Findings also indicated statistically significant differences in mean self-efficacy level scores for each of the 17 professional activities, but no overall significant differences in mean self-efficacy level scores based on selected demographic characteristics. Significant differences were found in the relationship between level of use and self-efficacy level for 15 professional activities. The most-mentioned challenges for faculty in using mLearning devices were the small screen size, connectivity issues, the incompatibility with Blackboard Learn, the on-screen keyboard, and the comparison to using a computer.