In this article, short carbon fibers (CFs) reinforced rigid polyurethane (RPU) composites were prepared with the aim of improving both strength and toughness. A tannic acid (TA)‐nickel (Ni) composite coating was spontaneously co‐deposited onto CFs surface by a one‐step electrodeposition method to strengthen the interface bonding of the composites. The satisfactory mechanical properties of the composites were mainly attributed to the superior interfacial adhesion. On the one hand, TA could play a role in refining Ni grain during electrodeposition. On the other hand, the hydroxyl groups attached to composite coating, which were introduced by TA, could react with the RPU matrix to form chemical bonds. When the composites were under stress, the chemical bonds could effectively transfer the stress from matrix to the interface, while the refined Ni crystals could greatly increase the stress transfer path, and thus improve the strength and toughness of the material. Compared with pure RPU, the tensile strength, bending strength,interlaminar shear strength, and impact strength of TA‐Ni‐coated CFs/RPU composites were improved by 14.8%, 83.1%, 28.7%, and 121.4%, respectively.