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Clearly, smartphone usage is increasing more than tablet usage, thus providing opportunities to evaluate how well the use of smartphones meets the requirements of patrons in an academic library setting. This study used the task-technology fit (TTF) model to explore the effectiveness of smartphones for interacting with online library systems, the need for smartphone support, and the “fit” of the device to tasks, as well as performance. The study used interviews and survey data to identify what are the core strengths and limitations of a smartphone construct that stimulate patrons to perform their tasks in an online library setting. Using exploratory factor analysis, preliminary findings confirmed Technology-Content, Technology-Ergonomics, Technology-Smartphone Support, Technology-Platform, and Technology-Interaction design as the core dimensions of the smartphone construct. The results of the structural model supported the overall TTF model in reflecting significant positive impact of task and technology in TTF for smartphones in a digital-library setting; it also confirmed a significant positive impact of TTF on individuals’ performance.