The aim of this study was to determine if there is a connection between the inquiry-based teaching of science in primary school and the development of the students' learning to learn competence. The research involved 333 fourth-grade students at primary schools in Croatia. The experimental research with parallel groups included a number of students who were exposed to inquiry-based teaching of science for three months, and a control group that was, at the same time, exposed to traditional instruction in the same curriculum content. The results of this research show that through inquiry-based teaching students developed a higher level of the learning to learn competence than by using traditional teaching methods. Therefore, it is recommended to use inquiry-based learning as often as possible, because by developing the students' learning to learn competence, students will be empowered for the process of lifelong learning.