<p>This study systematically investigates the effect of TiC content on the microstructure and properties of double-layer Ni60 + TiC composite coatings fabricated on 45 steel by laser cladding. The process parameters were optimized, and the coatings were characterized using SEM, EDS, XRD, microhardness testing, and friction–wear tests. Owing to the different thermal histories experienced by the upper and lower layers during double-layer cladding, distinct temperature gradients were generated, resulting in markedly different microstructural features between the two layers. Driven by buoyancy, TiC particles migrated upward and accumulated in the middle and upper regions. At a low TiC content of 10%, the coating hardness slightly decreased due to the dilution of solid-solution-strengthening elements in the Ni60 matrix. At 20% TiC, the coating exhibited the best overall performance, with a stable friction coefficient of 0.1 and wear resistance 5.06 times higher than that of the substrate, benefiting from the synergistic strengthening of dispersed TiC particles and in situ hard phases. At 30% TiC, although the hardness reached 1059.68 HV0.2, excessive TiC particles promoted oxidation to brittle TiO₂, which spalled under cyclic friction, leading to increased wear volume and fluctuating friction coefficients. Overall, an optimal TiC content of 20% provides an excellent balance between hardness and wear resistance, offering guidance for the composition design and process optimization of multilayer laser-clad nickel-based ceramic composite coatings.</p>