This chapter explores the potential of mobile cloud services to act as catalysts of pedagogical change in tertiary education. Mobile computing has emerged as a significant platform, with worldwide uptake dwarfing traditional desktop and laptop computing. According to the International Telecommunication Union (Acharya & Teltscher, 2010), at the end of 2010, 76% of the world’s population is now own mobile phones (116% in developed countries [by subscription], and 68% in developing countries), and mobile broadband subscriptions to the Internet (940 million) outnumbered fixed broadband connections (555 million). The advent of the iPhone, the iPad, and Android based smartphones have driven the explosion of mobile application development, numbering over 650,000 mobile apps across four main platforms (GSMArena, 2011; Perez, 2011), with many of these apps providing access and interaction with cloud services. Harnessing the potential of these two new computing behemoths within education is still at early stages of development and research. This chapter provides research-informed examples of the impact of mobile cloud services on teaching practice and learner experiences.