The improvement of comprehensive properties including hardness, toughness, wear, and adhesion strength of the coating-substrate system, especially avoiding the trade-off between the hardness and adhesion strength, is strongly required for various applications. Herein, an effective strategy is proposed, by in-situ solid-phase diffusion method, to fabricate a novel TiC–Fe gradient coating with high hardness and interfacial adhesion strength on cast iron. The eveloped coating was composed of equiaxed TiC particles and α-Fe phase. The microstructure was graded in TiC size and volume fraction. The formation of the graded microstructure was attributed to the nucleation-growth process controlled by diffusion of the carbon concentration gradient. The TiC volume fraction in the coating was as high as 95%. The phase interface (TiC/TiC interface and TiC/α-Fe interface) and the coating/substrate interface exhibited excellent interfacial bonding at the atomic scale. The novel gradient coating could simultaneously achieve high hardness (23.9 ± 1.3 GPa), high elastic modulus (265.7 ± 9.4 GPa), and excellent adhesion strength (>225 ± 10 MPa). Apparently, in-situ solid-phase diffusion method may provide a new route to fabricate TiC–Fe gradient coatings with high-volume fraction on steel/iron, capable of capable of exhibiting elevated hardness, high elastic modulus, excellent interfacial adhesion strength, and superior wear resistance.