New technology has been credited with the ability to extend human senses. However, adaptation and use of technology has been reported to be intricately mediated by usefulness and ease of use of technology among other contingencies. While Technology Acceptance Model (TAM) has provided the theoretical basis for adaptation and use of technology in a plethora of contexts, little, if any, study has examined the use of ubiquitous smart technological apparatus for academic purpose among the greatest adopters of the technology, university students. The current study examines students’ intention of smartphone adoption from the TAM perspective. Data has been collected from students in two public universities in Malaysia and Nigeria. IBM-SPSS version 20.0 and Structural Equation Modeling (SEM) approach with AMOS were used to analyze and test the hypothesized theoretical model. The results suggested that attitude, social influence and perceived usefulness were positively correlated with the respondents’ intention towards using smartphones for educational purposes. Moreover, students’ attitudes towards adoption of smartphones were directly predicted by perceived usefulness and directly self-efficacy, which in turn, had direct impact on students’ perceptions of easiness and usefulness. Findings made a considerable contribution to the heuristic value of TAM and facilitated the maximization of smart technologies for educational purposes.