Critical thinking (CT) is deemed an essential element of core competence in the 21st century. As science and technology advance and new technologies emerge, the prevalent use of smart classrooms in higher education offers a prime opportunity for fostering CT. However, the majority of current research on CT concentrates on traditional or fully online classroom settings, with scant attention given to the smart classroom context. To investigate the effects of smart classroom settings on college students’ CT, this study develops a model of influencing factors for CT within smart classroom environments, encompassing four elements: peer interaction (PI), learning engagement (LE), self-efficacy (SE), and preferences for the smart classroom learning environment (SCLE). Through a questionnaire survey, we analyzed the status quo and influencing factors of college students’ CT in smart classrooms. Results indicate that students’ CT generally exceeds the average level, suggesting a relatively high state of development of various abilities within the smart classroom environment. PI, LE, SE, and preferences for the SCLE significantly bolster the development of CT in college students. Based on these findings, this paper suggests strategies to refine college students’ CT within smart classroom settings, aiming to guide the cultivation of CT in higher education.