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This article explores Franz Brentano's opposition to papal infallibility, and sets this in the context of his development as a Catholic scholar. An active participant in the Catholic revival of the nineteenth century, Brentano contributed to the emergence of neoscholasticism through his philosophical rehabilitation of Aristotle. Brentano ultimately left the Church however as the result of intensive scrutiny of his faith occasioned by his analysis of infallibility. This article explores this crisis of faith by analyzing, for the first time, Brentano's position on papal infallibility, and suggesting ways that it informed his philosophical development.