The use of natural and non-natural play materials in early childhood education is a critical facilitator to children's learning and development. Different materials vary in their affordances for sophisticated play, imagination, and creativity, which contribute to children's complex thinking; with the current focus on technology, it has been suggested to balance its use with other materials. While childhood experiences with nature carry numerous benefits for development and complex thinking, most of the natural affordances have been documented in outdoor settings or with nature-based pedagogical approaches. The purpose, here, is to gain a better understanding of natural and non-natural material use across matched activities and approaches, in their affordances for preschool children's complex thinking during quality play. Using a cultural-historical interpretivist analysis of children's playful work and comments, findings indicated that both material types contributed to complex thinking, imagination, and creativity, but deeper connections and wider variety arose with natural materials. Findings suggest that teachers increase their use of natural materials in teaching, to help children develop deeper conceptual understandings and representations of their world.