Catalyst-referred etching (CARE) is a novel abrasive-free planarization method. CARE-processed 4H-SiC(0001) surfaces are extremely flat and undamaged over the whole wafer. They consist of single-bilayer-height atomic steps and atomically flat terraces. This suggests that the etching properties depend principally on the atomic-step density of the substrate surface. We used on-axis and 8 degrees off-axis substrates to investigate the processing characteristics that affect the atomic-step density of these substrates. We found a strong correlation between the removal rate and the atomic-step density of the two substrates. For the on-axis substrate, the removal rate increased with increasing surface roughness, which increases with an increasing atomic-step density. The removal rate ratio is approximately the same as the atomic-step density ratio of the two substrates.