The aim of this study was, for the first time, to measure and compare quantitatively the viscoelastic properties and surface roughness of coronary arteries. Porcine left anterior descending coronary arteries were dissected ex vivo. Viscoelastic properties were measured longitudinally using dynamic mechanical analysis, for a range of frequencies from 0.5 to 10 Hz. Surface roughness was calculated following three-dimensional reconstructed of surface images obtained using an optical microscope. Storage modulus ranged from 14.47 to 25.82 MPa, and was found to be frequency-dependent, decreasing as the frequency increased. Storage was greater than the loss modulus, with the latter found to be frequency-independent with a mean value of 2.10 ± 0.33 MPa. The circumferential surface roughness was significantly greater (p < 0.05) than the longitudinal surface roughness, ranging from 0.73 to 2.83 and 0.35 to 0.92 µm, respectively. However, if surface roughness values were corrected for shrinkage during processing, circumferential and longitudinal surface roughness were not significantly different (1.04 ± 0.47, 0.89 ± 0.27 µm, respectively; p > 0.05). No correlation was found between the viscoelastic properties and surface roughness. It is feasible to quantitatively measure the viscoelastic properties of coronary arteries and the roughness of their endothelial surface.