People’s opposition to vaccines can be difficult to overcome if their attitudes are motivated by psychological factors such as fears, ideological beliefs, and cognitive patterns, known as “attitude roots”. In this study, the objective was to identify which attitude roots are featured in individuals’ self-expressed reasons for negative vaccine attitudes, and explore how these are associated with psychological construct measures of those attitude roots. Our study involved12 556 participants from the US who wrote texts to explain their negative vaccine attitudes. The texts encompass 2,327 conceptually independent units of anti-vaccination argumentation, each coded for its attitude root(s) by at least two psychological experts. Each participant also completed scale measures of 11 psychological constructs and rated their agreement and familiarity with 11 anti-vaccination arguments, each representing an attitude root. We found that there were four groups of attitude roots whose self-expression was linguistically similar. Logistic regressions showed that a related psychological construct was the strongest, and significant, predictor for expression of three out of the four attitude root groups. In addition, latent class analysis of participants’ coded texts identified three distinct groups of participants that were characterised by their tendency to express combinations of arguments related to (1) fears, (2) anti-scientific conceptions, and (3) politicised perspectives. These findings are discussed in terms of how they can provide cues to vaccine communicators for how best to tailor messaging and responses to individuals motivated by different attitude roots, based on patterns in their self-expression.