Density functional theory and time-dependent density functional theory calculations provide pictures of the molecular orbitals involved in the ground and excited states of two cyano derivatives of 8'-apo-beta-caroten-8'-al synthesized via an acid-base-catalyzed Knoevenagel condensation reaction. Population analysis shows that the symmetry-allowed transition, S-0 ((1)A(g)) -> S-2 (B-1(u)) based on the C-2h symmetry is a HOMO (highest occupied molecular orbital) to LUMO (lowest unoccupied Molecular orbital) pi -> pi*, transition with electron densities located mostly on the polyene chain. Calculated and actual steady-state absorption spectra show similar features with low-energy peak maxima between 550 and 600 nm.