Melilite-type [A(2)](2)[B-I](2)[(B2O7)-O-II](2) gallates are promising ion conducting electrolytes for deployment in solid oxide fuel cells. Single crystals of [CaLa](2)[Ga](2)[Ga2O7](2), grown in an optical floating zone furnace, were investigated using a combination of transmission electron microscopy and single crystal X-ray diffraction. Strong anisotropic displacements of oxygen arise from the structural misfit between the interlayer Ca/La cations and the [Ga]-[Ga2O7] tetrahedral layers. A model employing two-dimensional modulation achieves bond lengths and bond angles that preserve satisfactory bond valence sums throughout the structure. The melilite belongs to the tetragonal superspace group P (4) over bar2(1)m(alpha, alpha, 0)00s((alpha) over bar, alpha, 0)000, alpha = 0.2160(5), with a subcell metric of a = 7.9383(2) angstrom, c = 5.2641(3) angstrom, onto which modulation vectors are superimposed: q(1) = alpha (a* + b*), q(2) = alpha (-a* + b*). Both displacive (cation and anion) and occupational (cation) modulations contribute to incommensuration. The analysis of structural adjustments that accompany changes in temperature and composition provides assurance that the crystal chemical model is correct. By better understanding the flexibility of this modulated structure a rational approach toward crystallochemical optimization of electrolyte performance by enhancing oxygen mobility becomes feasible.