Ni60 alloy is one of the important brands of nickel-based self-fusing alloys. It is widely used in industries such as metallurgy, mining, and other fields for the repair and protection of fragile parts. However, there is little literature on the effect of C content on its properties. In this study, two Ni60 alloy coatings with different C contents prepared by flame spraying and remelting were investigated by means of XRD, SEM, EBSD, friction wear testing, thermodynamic calculation, etc. The results showed that the calculated freezing range (FR) of Ni60 decreased from 983-1165.90 °C to 980-1154.28 °C and the melting range (MR) of Ni60 decreased from 966.27-1089.28 °C to 958.91-1045.41 °C when the C content increased from 0.72 wt.% (S1) to 1.01 wt.% (S2). Besides, the Cr7C3 phase size of the Ni60 layer increased with the increase of C addition. The coating shrinks during the remelting and solidification process, and the inner pores do not have sufficient time to escape, caused by the decreased FR, leading to the generation of holes and the degradation of surface quality in S2. However, the hardness of the S2 was 66 HV higher than that of S1, and the wear resistance of the S2 coating was superior as well because of more precipitated carbides therein. This work would give a hint at balancing the processability and mechanical properties for the development of high-performance coatings.