The paper presents an experimental study aiming to explore primary school students' response to Mobile Seamless Learning activities. The educational intervention and the consequent investigation were conducted in a suburban primary school in Greece, with second grade pupils, in the context of a learning subject entitled "Studying our Living Environment". The participant students (n = 14) engaged in both face-to-face (in-class, outdoor) and online (home) collaborative and individualistic activities supported by a variety of digital applications. Primary research data were gathered upon completion of the intervention via 5 group interviews and 12 individual interviews. The findings have shown that Mobile Seamless Learning can facilitate pupils' active engagement and improve their attitudes toward collaboration. Moreover, this approach can lead to the development of a learning community that promotes learners' motivation, enables them to construct new knowledge, and develop essential skills.