Assessment studies using structural equation modeling and Rasch Model have long been prominent in all areas of educational psychology. Their emphases have covered, but have not been limited to, the improvement of quality in teaching, learning, and research as well as the pursuit of research productivity. However, such methodological approaches have rarely taken place in the arena of information and communication technology (ICT) in tertiary education. As such, this study assesses Chinese lecturers’ expression of ICT satisfaction through the technology satisfaction model (TSM). Data from 196 Chinese lecturers were collected using stratified random sampling and analyzed applying structural equation modeling and the Rasch model. The findings suggested that Chinese lecturers’ satisfaction around ICT use was explored by the three underlying antecedents of computer self-efficacy, perceived usefulness, and ease of use. Computer self-efficacy was evidently a powerful exogenous variable in assessing direct and indirect causal associations among the dimensions of TSM. In future research, it is recommended that assessment of Chinese lecturers’ ICT use for teaching and research purposes should be considered through structural equation modeling and the Rasch model. This would support future researchers, academicians, and practitioners in performing technological measurements in all the arenas of tertiary education.