We sought to study the accuracy of dual-energy computed tomographic angiography (DE-CTA) for the assessment of symptomatic peripheral arterial occlusive disease of the lower extremity by using the dual-energy bone removal technique compared with a commercially available conventional bone removal tool. Twenty patients underwent selective digital subtraction angiography and DE-CTA of the pelvis and lower extremities. CTA data were postprocessed with two different applications: conventional bone removal and dual-energy bone removal. All data were reconstructed and evaluated as 3D maximum-intensity projections. Time requirements for reconstruction were documented. Sensitivity, specificity, accuracy, and concordance of DE-CTA regarding degree of stenosis and vessel wall calcification were calculated. A total of 359 vascular segments were analyzed. Compared with digital subtraction angiography, sensitivity, specificity, and accuracy, respectively, of CTA was 97.2%, 94.1%, and 94.7% by the dual-energy bone removal technique. The conventional bone removal tool delivered a sensitivity of 77.1%, a specificity of 70.7%, and an accuracy of 72.0%. Best results for both postprocessing methods were achieved in the vascular segments of the upper leg. In severely calcified segments, sensitivity, specificity, and accuracy stayed above 90% by the dual-energy bone removal technique, whereas the conventional bone removal technique showed a substantial decrease of sensitivity, specificity, and accuracy. DE-CTA is a feasible and accurate diagnostic method in the assessment of symptomatic peripheral arterial occlusive disease. Results obtained by DE-CTA are superior to the conventional bone removal technique and less dependent on vessel wall calcifications.