The mechanoluminescence of cerium (Ce) and terbium (Tb) lanthanide salts is studied in hydrocarbon [methane (CH ) and acetylene (C H )] and inert [helium (He), neon (Ne), argon (Ar), krypton (Kr), and xenon (Xe)] gaseous mixtures. The lines of *N , *Ln , inert gases, *CH, and *C radicals resulted from the mechanochemical decomposition of CH and C H are observed in the emission spectrum. The luminescence intensity of the inert gases decreases with the hydrocarbon gas concentration in the mixture. The intensities of the *CH or *C bands remains almost unchanged within 15-100 vol% of CH or C H in the mixture. When the concentration of CH or C H is lower than 15%, the intensities of the CH or C bands increase achieving their maxima at 0.5-3% of the hydrocarbon. This is probably due to the optimal compositions of the mixtures with the most efficient generation of electrical discharges responsible for mechanoluminescence.