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We describe and analyze the selective (resonance) laser-induced initiation of chemical decomposition reactions in PETN and propose a potential mechanism of the phenomenon. Based on our experiments, the photoinitiation of PETN is a two-stage process that is comprised of a laser-induced optical excitation of the molecule with the activation energy of 1.17 eV (1060 nm) by neodymium phosphate glass laser followed by the thermal decomposition of the excited state with the energy barrier of 0.4 eV. We also illustrate that the small efficiency of the optical absorption of PETN at this wave length can be enhanced by the MgO light scattering additives, which significantly increase the absorption due to multiple scattering incidents in PETN. The discovered resonance photoinitiation clearly demonstrates a strategy for designing tunable explosive material systems and identifies ways to control sensitivity of the materials to rapid decomposition.