We report the anisotropic atomic expansion dynamics of multi-walled carbon nanotubes, using 4D electron microscopy. From time-resolved diffraction on the picosecond to millisecond scale, following ultrafast heating at the rate of 10 13 K/s, it is shown that nanotubes expand only in the radial (intertubule) direction, whereas no significant change is observed in the intratubular axial or equatorial dimensions. The non-equilibrium heating occurs on an ultrafast time scale, indicating that the anisotropy is the result of an efficient electron-lattice coupling and is maintained up to equilibration. The recovery time, which measures the heat dissipation rate for equilibration, was found to be on the order of ∼100 μs. This recovery is reproduced theoretically by considering the composite specimen-substrate heat exchange.