A systematic study of the synthesis-structure-mechanical properties re
lationship is reported for MoSi2Nx films. MoSi2Nx films with nitrogen
content x ranging between 0 and 4.2 were prepared by sputtering techni
que. Cross-sectional transmission electron microscopy was used to exam
ine the as-sputtered and annealed microstructures when exposed to diff
erent annealing conditions. Nanoindentation was employed to characteri
ze the mechanical response of the materials as a function of the struc
tural changes. As-sputtered MoSi2Nx films exhibit an amorphous structu
re. Annealing at 900 degrees C causes different microstructural change
s depending on the nitrogen content. The resulting microstructure cons
ists of nanocrystalline C11(b)-MoSi2 for x=0, nanocrystalline C40 phas
e for x=1.5 and amorphous for x=2.95 and 4.2. The hardness of the as-s
puttered MoSi2Nx films increases with nitrogen content to a maximum of
17.8 GPa (x similar to 3) and then decreases for higher nitrogen cont
ents. Annealing at 500 degrees C and 900 degrees C, respectively, resu
lts in an increase in hardness. The rate of increase decreases with in
creasing nitrogen concentration. Increase in modulus is strongly relat
ed to the crystallization process, which is also affected by the nitro
gen content in the MoSi2Nx films. These results suggest the possibilit
y of engineering MoSi2Nx by varying the composition and heat treatment
to produce suitable materials properties for different materials appl
ications.