In this study, we present a number of experiments on the transformation of graphite, diamond, and multiwalled carbon nanotubes under high pressure conditions. The analysis of our results testifies to the instability of diamond in the 55–115 GPa pressure range, at which onion-like structures are formed. The formation of interlayer sp3-bonds in carbon nanostructures with a decrease in their volume has been studied theoretically. It has been found that depending on the structure, the bonds between the layers can be preserved or broken during unloading.