We have studied the kinetic and photoinduced aspects of the transformation of the cluster structure of ultrahard fullerite in the pressure ranges of a new phase diagram of carbon corresponding to the stability regions of diamond (up to 55 GPa) and onion-like structures of the fullerene type (55–115 GPa). A long exposure (for 3 months) at 25 GPa leads to the beginning of the transformation of the sample of ultrahard fullerite into diamond. A further increase to 70 GPa, under the influence of laser irradiation at wavelengths of 405 and 532 nm at doses of 5*1013 J/m2, initiates the formation of onion-like particles in ultrahard fullerite samples, which is accompanied either by a broadening of the high-frequency mode of the Raman spectrum, or its disappearance under high pressure. After pressure release, the high frequency mode of the Raman spectrum is located at 1570–1605 cm−1 at excitation wavelengths of 532 and 405 nm, respectively, which is typical for ultrahard fullerite. Bulk modulus of such an irradiated sample corresponds to a typical value for ultrahard fullerite of about 600 GPa. In addition to the formation of nanodiamonds and onion–like particles, the synthesis of ultrahard fullerite is also accompanied by the appearance in the sample of systems with double bonds of the C=C=C type with a line around 1935 cm−1, the nature of which is not entirely clear.