Multicomponent and high-boron cast alloys have been recognized as materials with excellent wear resistance due to the formation of hard phases called carbides and borides. However, the wear performance of the combination of these two materials called hybrid multicomponent cast alloys (HMCAs) has not been comprehensively studied. Therefore, this study will evaluate the effect of C (0–0.9 wt.%) and B (1.5–3.5 wt.%) addition on the erosion wear behavior of an HMCA containing 2.5 wt.% Ti, 10 wt.% Cr, and 5 wt.% each of V, Mo, and W. Shot-blast erosion testing was used to evaluate the wear resistance of each alloy. The test was conducted for 3600 s using 2 kg of irregularly shaped steel sand as a scraper at impact angles of 30°, 60°, and 90°. The results showed that the highest wear rate in 0C and 0.45C with 1.5–3.5% B occurred at an impact angle of 60° due to gouging and indentation mechanisms occurring simultaneously. However, different results occurred in the case of 0.9C with the same amount of B where the wear rate increased with increasing impact angle due to brittleness. Based on the chemical composition, the wear resistance of the alloy increased with increasing C content due to higher hardness values. However, the reverse performance occurred when the addition of B exceeded the threshold (more than 1.5 wt.%) despite the higher hardness. This fact was due to the susceptibility to carbide cracking as the amount of B increased. Therefore, the alloy with the best erosion wear resistance was 0.9C–1.5B HMCA.