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This paper concentrates on the deformation behavior of amorphous diamondlike carbon composite materials. Combined nanoindentation and ex situ cross-sectional transmission electron microscopy investigations are carried out on TiC/a-C nanocomposite films, with and without multilayered structures deposited by pulse dc magnetron sputtering. It is shown that by controlling the distribution of nanocrystallites forming nanoscale multilayers, the system can be used as a “microstructural ruler” that is able to distinguish various deformation patterns, which can be hardly detected otherwise in a homogeneous structure. It is shown that rearrangement of nanocrystallites and displacement of a-C matrix occur at length scales from tens of nanometer down to 1 nm. At submicrometer scale homogeneous nucleation of multiple shear bands has been observed within the nanocomposites. The multilayered structure in the TiC/a-C nanocomposite film contributes to an enhanced toughness.