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Lithiation of individual multiwalled carbon nanotubes (MWCNTs) was conducted in situ inside a transmission electron microscope. Upon lithiation, the intertube spacing increased from 3.4 to 3.6 Å, corresponding to about 5.9% radial and circumferential expansions and ∼50 GPa tensile hoop stress on the outermost tube wall. The straight tube walls became distorted after lithiation. In situ compression and tension tests show that the lithiated MWCNTs were brittle with sharp fracture edges. Such a failure mode is in stark contrast with that of the pristine MWCNTs which are extremely flexible and fail in a “sword-in-sheath” manner upon tension. The lithiation-induced embrittlement is attributed to the mechanical effect of a “point-force” action posed by the intertubular lithium that induces the stretch of carbon–carbon bonds in addition to that by applied strain, as well as the chemical effect of electron transfer from lithium to …