Introduction: The rise in the unemployment rate that accompanied the 2008 economic crisis is associated in France with an increase in the suicide rate. The objective of this study was to estimate the ecological association, by sex and age, between suicide and unemployment rates in metropolitan France between 2000 and 2010. Methods: The statistical analyses used a quasi-Poisson model. The dependent variable was the suicide rate; the independent variable was the unemployment rate. This model was adjusted for age, sex, region of residence, quarter of death, and a linear temporal trend. The age groups 15–24, 25–49, 50–64, and 65+ were studied. Results: For a 10% increase in the unemployment rate, the suicide rate for all genders combined increased significantly by 1.5% (95% CI: [0.7–2.3%]). This association remained significant only among men (1.8% increase [0.9–2.7%]), particularly men aged 25–49 (2.6% increase [1.3–3.9%]). Conclusion: The association observed in France between suicide rates and unemployment rates particularly affects men of working age. Suicide prevention initiatives targeting the working-age population should prioritize young men.