The invention relates to a method for producing nanometric layers with content of diamond or fullerene nanoparticles, by irradiation with ultrashort pulses within the range of picoseconds and femtoseconds, generated by high power lasers (terawatt – TW or petawatt – PW) and, in particular, to a process of forming diamond/fullerene structures on layers of interest for the nuclear fusion, namely C, Be and W layers. According to the invention, the method of modifying a layer deposited on a graphite sublayer consists in producing, by the thermionic vacuum arc method, a C and W bi-layer with the W layer thickness ranging between 2000…2500 nm and that of the C layer ranging between 180…200 nm, deposited on a parallelepipedal graphite sublayer, guiding some laser beams of short duration 100…300 ps in mono-pulse or multi-pulse, with peak power within the range 10…10watt, with pulse energies in the range of micro-Joule to milli-Joule, by means of a lens, in a focal point having the size of 20 x 2 mm, in order to form, by multi-photon absorption, diamond nanocrystals embedded in an amorphous C matrix. As claimed by the invention, the method of modifying a film deposited on a Si sublayer consists in producing, by the thermionic vacuum arc method, a C, Be and W mixed film on Si sublayer, guiding some laser beams of short duration 100 fs…360 ps in mono-pulse or multi-pulse with peak power within the range of 10…10watt, with pulse energies in the range of micro-Joule to milli-Joule, by means of a condensing lens, in a focal point of a plasma, at the normal pressure of the environment or deuterium at the pressure of 20 mbar, in order to produce structures with content of fullerene, beryllium oxide and/or wolfram oxide.