In this study, multicomponent alloy fillers were deposited on low-carbon steel substrates using gas tungsten arc welding (GTAW) process. The microstructure and wear properties of Al-Co-Cr-Ni-Mo-Fe-Si multicomponent alloys were studied. The GTAW cladding layers were analyzed by X-ray diffraction (XRD), field-emission scanning electron microscopy (FE-SEM), X-ray energy dispersive spectroscopy (EDS), and transmission electron microscope (TEM). The results show that the microstructure mainly consisted of dendritic FeMoSi and interdendritic BCC phases and that the addition of Si coarsened the primary FeMoSi phase. In addition, different precipitate morphologies were found in the interdendrites. As the Si content increased from 5.92 to 14.53 at%, the microhardness also increased from 826 to 885 Hv and the wear resistance improved significantly. The FeMoSi dendrites possessed covalent-dominant strong atomic bonds that enhanced the hardness and wear resistance of claddings.