Despite chemistry’s recognized importance to multiscale industrial and environmental processes, first-year undergraduate chemistry is often regarded as comprising a collection of unconnected topics with little relevance to everyday life. Implementing systems thinking into the chemistry curriculum can help to contextualize chemistry learning and increase chemistry’s relevance to students. In this study, we designed, implemented, and evaluated the use of authentic learning activities featuring concepts of green chemistry and sustainability to introduce first-year undergraduate chemistry students to systems thinking. The intervention was evaluated using a mixed methods approach to assess participants’ systems thinking skills and measure motivations and attitudes toward chemistry. Thematic analysis of learning activity assessments revealed that participants were able to demonstrate systems thinking skills in a variety of chemistry-related sustainability contexts. Quantitative analysis of survey responses showed participants reported variable levels of motivation and attitudes toward chemistry learning, while qualitative analysis of semistructured interviews revealed the learning activities improved participants’ motivations and attitudes toward learning chemistry and understanding chemistry’s role in solving sustainability challenges. Our results can be used to inform future design and delivery of modernized chemistry curricula.