The time children spend with mobile devices has increased in recent years. Preschoolers’ home usage of mobile devices has mainly been investigated through parents’ perceptions. Listening to the children’s voices can help us understand this matter more directly. Therefore, in this study, a convergent mixed methods approach was employed to help us investigate the home usage of mobile devices by young children, focusing on children’s comments. The participants were 55 Greek children aged 4–6, attending two public kindergartens in Patras. Children described in detail their activities on mobile devices, through semi-structured interviews. The results indicated that the most popular activity for the children was playing digital games. The children were able to demonstrate and describe activities for educational purposes (letters, numbers, digital puzzles, documentaries, etc.) during the home usage of mobile devices. The circumstances in which they are allowed to use their mobile devices is when their parents want to keep them calm during quiet hours or in public places. Implications for introducing mobile learning activities in Greek education are discussed.