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Ambitious entrepreneurship is rare but its economic impact is far stronger than that of less or nonambitious entrepreneurial activity. Current research in this emergent field of inquiry focuses on a declarative ambition, an intention, or a motivation to grow, and it essentially examines its effects on the short-term, finding mixed results. Building on the theory of planned behavior and the concept of sustainable growth, we introduce the notion of ambitious behavior to describe the realization of an intention of ambition. We then test for the impact of ambitious behavior on ambition realization, defined as high growth, on a sample of 1,970 European SMEs. We find a significant positive relationship. We also test for the possible moderating effects on this relationship of the presence of external investors, the presence of an entrepreneurial team, an entrepreneurial management style, and environmental dynamism. We find significant results, albeit counterintuitive ones. We make multiple contributions: theoretical (to the literatures on SMEs growth and ambitious entrepreneurship), methodological (mainly based on our measurement of ambitious behavior), and practical (notably with regard to public policies).