The purpose of this research is to investigate the effect of using argumentation and problem-based learning approaches on the development of environmentally responsible behaviours among pre-service science teachers. Experimental activities were implemented for 14 weeks for 52 class hours in an environmental education class within a science teaching department. A mixed method was used as a research design; particularly, a special type of Concurrent Nested Strategy was applied. The quantitative portion was based on the one-group pre-test and post-test models, and the qualitative portion was based on the holistic multiple-case study method. The quantitative portion of the research was conducted with 34 third-year pre-service science teachers studying at a state university. The qualitative portion of the study was conducted with six pre-service science teachers selected among the 34 pre-service science teachers based on the pre-test results obtained from an environmentally responsible behaviour scale. t tests for dependent groups were used to analyse quantitative data. Both descriptive and content analyses of the qualitative data were performed. The results of the study showed that the use of the argumentation and problem-based learning approaches significantly contributed to the development of environmentally responsible behaviours among pre-service science teachers.