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The purpose of this survey study is to investigate the relation between Head Start teachers’ science teaching attitude and self-efficacy. A total of 150 participants from eight states completed online survey questionnaires regarding their science teaching attitudes and self-efficacy. Data were analyzed using a multilevel regression approach. Results indicated that Head Start teachers who perceived fewer challenges, a higher level of comfort, and more benefits in teaching science tended to be more confident in their abilities to teach science but not in their expectations of teaching effectiveness. This finding pointed to the need to enhance Head Start teachers’ science teaching efficacy by mitigating challenges, elevating the level of comfort, and recognizing the value of teaching science to young children.