By making use of the diagonalization of the complete d3 energy matrix in a trigonally distorted cubic-field and the theory of pressure-induced shifts (PS) of energy spectra, the whole energy spectrum of α-Al2 O3 :Mn4+ and PS of levels have been calculated. All the calculated results are in excellent agreement with the experimental data. The comparison between the results ofα-AlO3:Mn4+ and ruby has been made. It is found that on one hand, R1-line and R2line PS of α-Al2O3:Mn4+ and ruby are linear in pressure over 0 ～ 100 kbar, and their values of the principal parameter for PS are very close to each other. On the other hand, the sensitivities of R1-line and R2-line PS of α-Al2O3:Mn4+are higher than those of ruby respectively, which comes mainly from the difference between the values of parameters at normal pressure of two crystals; moreover, the expansion ofd-electron wavefunctions of α-Al2 O3 :Mn4+ with compression is slightly larger than the one of ruby, and the effective charge experienced by d-electrons of α-Al2O3:Mn4+ decreases with compression more rapidly than the one of ruby. In the final analysis, all these can be explained in terms of the facts that the two crystals are doped α-Al2O3 with two isoelectronic ions; the strengths of the crystal field and covalency of α-Al2O3 :Mn4+ are larger than those of ruby respectively, due to the charge of Mn4+ to be larger than that of Cr3+.