With the emerging technologies of augmented reality (AR) and virtual reality (VR), the learning process in today’s classroom is much more effective and motivational. Overlaying virtual content into the real world makes learning methods attractive and entertaining for students while performing activities. AR techniques make the learning process easy, and fun as compared to traditional methods. These methods lack focused learning and interactivity between the educational content. To make learning effective, we propose to use handheld marker-based AR technology for primary school students. We developed a set of four applications based on students’ academic course of primary school level for learning purposes of the English alphabet, decimal numbers, animals and birds, and an AR Globe for knowing about different countries around the world. These applications can be played wherever and whenever a user wants without Internet connectivity, subject to the availability of a tablet or mobile device and the required target images. These applications have performance evaluation quizzes (PEQs) for testing students’ learning progress. Our study investigates the effectiveness of AR-based learning materials in terms of learning performance, motivation, attitude, and behavior towards different methods of learning. Our activity results favor AR-based learning techniques where students’ learning motivation and performance are enhanced compared to the non-AR learning methods.