Recently, there has been a transition from traditional paper or computer-based learning environments to smartpad-based learning environments, which are based on touch and involve various cognitive strategies such as touch operation and note taking. Accordingly, the use of smartpads can provide an effective learning environment through cross-modality, which simultaneously integrates information using two or more sensory modalities. Based on this rationale, this study investigated the effects of cross-modality (vision and tactility) on knowledge acquisition in a smartpad-based learning environment. Interaction between different modalities and learners' self-regulated learning (SRL) skills was also tested. Ninety-nine college students were randomly assigned to three different learning environments: paper-based, smartpad-based unimodal, and smartpad-based cross-modal environments. Students were differentiated according to high and low SRL skill levels. The findings suggest that the participants in the smartpad-based cross-modal environment significantly outperformed the participants in the smartpad-based unimodal environment pertinent to identification and comprehension knowledge acquisition. Furthermore, the participants in the smartpad-based cross-modal environment performed equally with the participants in the paper-based environment.