Though the use of mobile devices (eg, tablets, smartphones) by young children is pervasive and increasing, research relating children's use of mobile devices to their development is only beginning to emerge. Learning, language development, and self-regulation skills among children aged 0 to 5 are of particular interest to pediatric clinicians, researchers, parents, and policymakers, as these skills foreshadow important outcomes across the lifespan. Experimental research reviewed herein suggests that the interactivity allowed by mobile devices has benefits over passive viewing (for example, of television) for young children's learning and self-regulation, but studies of naturalistic use suggest increased use of mobile devices is associated with poorer language and self-regulation. Pediatric clinicians can be important sources of support for families endeavoring to navigate their children's use of mobile devices by providing advice and resources, such as communicating reasonable time limits and sharing sources of developmentally appropriate content. Future research should implement innovative, rigorous research designs and methods to clarify mechanisms underlying potential negative effects of naturalistic use of mobile devices by young children and investigate how content and context of young children's mobile-device use may influence relations between such use and children's skills.