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Mechanical properties and glass transition temperatures
(
T
g
)
of Fe-Cr-Mo-P-C-B bulk metallic glasses containing up to
27
at.
%
metalloids have been studied. The shear modulus
(
G
)
is found to decrease with increasing metalloid content and a maximum plastic strain of
∼
3
%
is obtained, despite the increase in the number of strong metal-metalloid bonds. Also,
T
g
increases with the decrease in
G
, in contrast to usual behavior. By employing first-principles calculations, the results are discussed in light of atomic bonding and connectivity in the amorphous network. The findings are relevant to understanding ductility and glass transition of metallic glasses.