Аннотация:The ultrashort-laser photoexcitation and structural modification of buried atomistic opti-cal impurity centers in crystalline diamonds are the key enabling processes in the fabrication of ultrasensitive robust spectroscopic probes of electrical, magnetic, stress, temperature fields, and sin-gle-photon nanophotonic devices, as well as in “stealth” luminescent nano/microscale encoding in natural diamonds for their commercial tracing. Despite recent remarkable advances in ultrashort-laser predetermined generation of primitive optical centers in diamonds even on the single-center level, the underlying multi-scale basic processes, rather similar to other semiconductors and dielec-trics, are almost uncovered due to the multitude of the involved multi-scale ultrafast and spatially inhomogeneous optical, electronic, thermal, and structural elementary events. We enlighten non-linear wavelength-, polarization-, intensity-, pulsewidth-, and focusing-dependent photoexcitation and energy deposition mechanisms in diamonds, coupled to the propagation of ultrashort laser pulses and ultrafast off-focus energy transport by electron–hole plasma, transient plasma- and hot-phonon-induced stress generation and the resulting variety of diverse structural atomistic modifi-cations in the diamond lattice. Our findings pave the way for new forthcoming groundbreaking experiments and comprehensive enlightening two-temperature and/or atomistic modeling both in diamonds and other semiconductor/dielectric materials, as well as innovative technological break-throughs in the field of single-photon source fabrication and “stealth” luminescent nano/microen-coding in bulk diamonds for their commercial tracing.