The structures of pyrene-based organic light-emitting diode materials were optimized, and their molecular orbitals, light absorption, and emission wavelength were predicted using density functional theory calculations with five different functionals: r2SCAN, B3LYP, M06-2X, CAM-B3LYP (한글요약문과 용어 통일 필요), and wB97X. Additionally, the study examined trends in the results based on the different calculation methods and identified suitable functional-basis set combinations through comparison with experimental values. The four selected luminescent materials were substituted with bulky groups such as m-terphenyl and triphenylbenzene on the pyrene chromophore to prevent stacking of the pyrene, thereby suppressing the transition state caused by intermolecular interactions and preventing a reduction in luminescence efficiency. The qualitative trends from the calculations mostly matched the experimental results, with the B3LYP-D3/def2-QZVP method providing the closest agreement with experimental values, particularly in terms of absorption and emission wavelengths.