If the implementation of blended and mobile learning across disciplines is to be maximized, it is important for researchers to understand how students perceive and use wireless handheld devices, in order to build on those current practices and help to facilitate the next level of adoption. To enhance that understanding, this chapter analyzes data from 228 survey questionnaires conducted in October and November 2008. Students were enrolled in two faculties at the authors’ institution. Questions explored students’ views and opinions about the uses of wireless handheld devices, such as personal digital assistants, handheld PCs, and smart phones, for teaching and learning activities. The chapter draws on a case study method using factor and regression analysis to interpret the questionnaire responses about the uses of wireless handheld devices in higher education. The principal findings included that behavior and attitude contribute strongly to the perceived performance of using such devices in the chosen context, and that facilitating conditions have a more complex and mediated relationship with behavior and attitude on the one hand and perceived performance on the other. The authors elaborate the implications of those findings for increasing alignment across several different interfaces related to blended and mobile learning in the early 21st century.