A single‐crystal graphene film grown on a Cu(111) foil by chemical vapor deposition (CVD) has ribbon‐like fold structures. These graphene folds are highly oriented and essentially parallel to each other. Cu surface steps underneath the graphene are along the <110> and <211> directions, leading to the formation of the arrays of folds. The folds in the single‐layer graphene (SLG) are not continuous but break up into alternating patterns. A “joint” (an AB‐stacked bilayer graphene) region connects two neighboring alternating regions, and the breaks are always along zigzag or armchair directions. Folds formed in bilayer or few‐layer graphene are continuous with no breaks. Molecular dynamics simulations show that SLG suffers a significantly higher compressive stress compared to bilayer graphene when both are under the same compression, thus leading to the rupture of SLG in these fold regions. The fracture strength of a CVD‐grown single‐crystal SLG film is simulated to be about 70 GPa. This study greatly deepens the understanding of the mechanics of CVD‐grown single‐crystal graphene and such folds, and sheds light on the fabrication of various graphene origami/kirigami structures by substrate engineering. Such oriented folds can be used in a variety of further studies.