High chromium and nickel indefinite chilled cast iron (ICCI), as an excellent hot roll material, is the preferred roll variety due to its good combination of surface roughness, hot crack resistance, and hot wear resistance. The microstructure and hardness of ICCI roll materials with different contents of (NbTi)C particles is studied here, and the microstructure evolution process is analyzed by X-ray diffraction. The influence of (NbTi)C particles on the carbide morphology and distribution is investigated by metallographic microscopy and scanning electron microscopy, and the existence of (NbTi)C particles is observed. The experimental results show that (NbTi)C particles are present in granular, rod, and polygonal forms. Combined with a Thermo-Calc solidification phase diagram, it is found that the (NbTi)C particles undergo eutectic precipitation in the melt, forming short rod-shaped (NbTi)C carbides with a size of about 10 μm. Through the Rockwell hardness test, it is found that the hardness after adding 0.8 wt % (NbTi)C particles was 54.4 HRC, which was 21.1% higher than that without the addition.