We report an electro-enhanced catalytic etching approach for direct atomic-level patterning of single-crystal 4H-SiC (0001) surfaces. The process utilizes platinum-coated probes under a negative sample bias, which enhances catalytic reactions and promotes etching of SiC without additional mechanical load. Unlike traditional etching approaches that rely on hazardous chemicals such as hydrofluoric acid, this approach operates under ambient conditions, offering improved safety and environmental compatibility. High-angle annular dark field scanning transmission electron microscopy images reveal that the etched regions retain the perfect crystallographic order down to the outermost atomic layer, with no detectable subsurface damage. The electro-enhanced catalytic etching approach demonstrated here could be extended to fabrication of other semiconductor materials, driving advancements in microelectronics, quantum information, and integrated optoelectronics.