Background To study the association between the total plasma homocysteine (tHcy) concentration and the carotid artery intima-medial wall thickness (IMT), pulse wave velocity (PWV) and the presence of arterial plaques in a French population. Methods Cross-sectional analysis of data from 556 male and 559 female middle-aged participants (mean (± SD) age 59.6 ± 4.7 years) provided by an ongoing intervention trial. Results Mean geometric tHcy concentration was higher for men than for women (10.6 vs. 8.5 μmol/L, p < 0.001) and was associated in the expected direction with known determinants. The mean IMT was 0.71 ± 0.1 mm for men and 0.69 ± 0.1 mm for women ( p < 0.001), the mean PWV was, respectively, 12.0 ± 2.8 and 10.9 ± 2.2 m/sec ( p < 0.001), and the percentages of subjects with plaques were, respectively, 40.8% and 22.7% ( p < 0.001). In men only, the age-adjusted mean IMT and PWV increased with an increasing tHcy concentration: the IMT was 0.71 mm in the first tHcy-quartile and 0.73 mm in the fourth tHcy-quartile ( p for linear trend = 0.03), the PWV values were, respectively, 11.6 and 12.4 m/sec ( p for linear trend = 0.01). These associations disappeared after adjustment for conventional cardiovascular disease risk factors. Conclusion In this population, the tHcy concentration was not associated with measures of arterial thickness and stiffness.