This paper presents obtaining a single-phase ferrite layer with low content of carbon (the average thickness is about 156–246 µm) on the surface of 0.45% carbon steel by precisely designing the cooling rate during heat treatment, and its mechanical properties show a graded change in the cross-section. It may be achieved by preparing gradient/multilayer materials with more commonly utilized structures or a specific performance. Combining with phase identification by employing electron backscatter diffraction (EBSD) of the layer in this study is BCC ferritic phases. Based on the examination of Continuous Cooling Transformation (CCT) curves, the following conclusions are given. Under the cooling process with gradient temperature, a ferrite layer first forms on the outer lower temperature surface of the 0.45% carbon steel and subsequently develops by pushing the surplus carbon to the inner higher temperature austenite region. It is corroborated by the experimental findings of carbon contents dispersion acquired by electron probe microanalyzer (EPMA). Finally, the experimental findings of grain orientations and size distribution defined by electron backscatter diffraction (EBSD) are given as requirements for microscopic interpretation of the combination of excellent strength and bending capabilities of materials. Furthermore, the experimental findings of oxidation precisely specified the cooling rate during heat treatment of Cu coating samples, which are defined as criteria for identifying the production mechanism of the surface ferrite layer. It provides a theoretical explanation and direct experimental proof for creating the ferrite layer on the surface.