Purpose: To determine whether higher concentrated gadolinium chelates are advantageous for the recently introduced concept of total-body magnetic resonance angiography (MRA), allowing whole-body coverage, extending from the carotid arteries to the runoff vessels, in merely 72 seconds. Materials and Methods: Total-body three-dimensional (3D) MRA using a 1 M Gd-chelate (gadobutrol, Gadovist®, Schering, Berlin, Germany) at a dosage of 0.2 mmol/kg body-weight (biphasic injection protocol: 1.3 mL/second and 0.7 mL/second) was performed on three healthy volunteers and ten consecutive patients with DSA-documented peripheral vascular disease. Separated by at least 72 hours, the three healthy volunteers also underwent the same MRA-protocol, using gadopentetate dimeglumine in equimolar dosages. Results: Compared to equimolar dosages, mean signal-to-noise ratio (SNR) and contrast-to-noise ratio (CNR) values in the three volunteers were significantly higher (up to 32.5% for the arteries of the thighs and calves) using gadobutrol. In the ten patients, gadobutrol-based total-body MRA accurately assessed significant stenoses (luminal narrowing > 50%) with sensitivities and specificities of 96.2% (95% CI 0.83-0.97) and 95.7% (95% CI 0.84-0.96), respectively, compared to digital subtraction angiography. Conclusion: The MRA image quality for total-body MRA provided by the administration of gadobutrol is superior to that obtained following administration of an identical dose of gadopentetate dimeglumine, and therefore shows promise for use as a comprehensive single exam assessing the entire arterial system for the presence of atherosclerotic disease manifestations.