While carbon capture and storage (CCS) is considered to be critical to achieving long-term climate-protection goals, public concerns about the CCS practice could pose significant obstacles to its deployment. This study reports findings from the first state-wide survey of public perceptions of CCS in a coal-intensive state, with an analysis of which factors predict early attitudes toward CCS. Nearly three-quarters of an Indiana sample (N = 1001) agree that storing carbon underground is a good approach to protecting the environment, despite 80% of the sample being unaware of CCS prior to participation in the two-wave survey. The majority of respondents do not hold strong opinions about CCS technology. Multivariate analyses indicate that support for CCS is predicted by a belief that humankind contributes to climate change, a preference for increased use of renewable energy, and egalitarian and individualistic worldviews, while opposition to CCS is predicted by self-identified political conservatism and by selective attitudes regarding energy and climate change. Knowledge about early impressions of CCS can help inform near-term technology decisions at state regulatory agencies, utilities, and pipeline companies, but follow-up surveys are necessary to assess how public sentiments evolve in response to image-building efforts with different positions on coal and CCS.