Nickel silicon carbide (Ni-SiC) nanocomposite coatings are extensively used in the engineering field due to their exceptional mechanical characteristics. In this study, pulsed electrodeposition from a nickel Watts bath on a cast iron (CI) cylinder liner produced a Ni-SiC nanocomposite coating. The current study concentrated on multi-objective optimization to maximize microhardness and minimize surface roughness of the composite coating by grey relational analysis (GRA) and the contribution of coating parameters was analyzed by analysis of variance (ANOVA). The GRA-ANOVA-ANOVAt shows that the effects of the square term of duty cycle (Y2), the linear term of current density (Z), and the square term of frequency (X2) are most significant and affect the coating characteristics at a 95% confidence level. The inclusion of SiC particles altered the preferred coating crystallographic orientation from (200) to (111). The optimal coating parameters of frequency 100 Hz, duty cycle 80%, and current density 0.5 A/cm2 produced the best mechanical properties for Ni (79.38 wt%), Si (0.76 wt%), and C (19.86 wt%). According to the ANOVA, the linear term of current density (Z) and the quadratic terms of duty cycle (Y2) and frequency (X) have a significant influencing role with contributions of 27.74, 24.18, and 22.90%, respectively. EDX analysis of the Ni-SiC coating showed that carbon is the dominant element, comprising 54.52 wt. % and 19.86 wt. %, followed by nickel and silicon.