For enhancing wear property of Fe-based bulk amorphous alloys as structural materials, We investigate effects of Cr or Mo compositions on wear and mechanical behaviors of FeCSiBPMo and FeCSiBPAlCr system bulk amorphous alloys which are suction-cast into a copper mold by arc melting in an argon atmosphere using a suction casting technique. X-ray diffraction, differential scanning calorimeter and Scanning electron microscopy were used to observe the microstructure and surface morphologies. Cr-Fe or Mo-Fe substitutions led to a dramatic increase in the glass transition temperature as well as the supercooled liquid region. After the wear test, the mass loss of both BAAs decreased remarkably at higher element. Nanoindentation results indicate that with an increase of the Cr or Mo compositions, the hardness and elastic modulus increased in both BAA samples. These results suggest that wear behaviors of the BAAs corresponded to change in hardness, which means that fracture morphologies of worn surface are strongly dependent on surface hardening with high Cr or Mo content.