Compact and continuous Ni‐coated zirconium oxide‐toughened alumina (ZTA) particles (ZTAp@Ni) and CuNi‐coated ZTA particles (ZTAp@CuNi) are prepared by electroless deposition. The thicknesses of the Ni and CuNi coatings are 6.84 and 21.35−43.10 μm, respectively. The ZTAp@Ni‐ and ZTAp@CuNi‐reinforced high‐chromium cast iron (HCCI) composites are fabricated by nonpressure cast‐infiltration method. Results show that compact interfacial bonding is formed in S3′‐ZTAp@CuNi/HCCI without any casting defect. The addition of Ni element can effectively improve the amount of (Cr,Fe)7C3 and refine the grains in HCCI matrix, and Cu element can improve the strength and toughness of the matrix. The compression performance testing shows that the compressive strength and yield strength of S3′‐ZTAp@CuNi/HCCI are up to 1128.03 and 1049.40 MPa, respectively. In addition, three‐body abrasive testing demonstrates that the abrasive wear resistance of the S3′‐ZTAp@CuNi/HCCI is optimal. This can be attributed to the compact combination between ZTAp@CuNi and HCCI matrix, which benefits the load transfer and the protection of ZTA particles to avoid brittle fracture and debonding. So, the appropriate additions of Cu and Ni elements, that is, the thickness and content control of CuNi coatings on ZTA surfaces, are very crucial for the performance improvement of composites.