There is a heavy emphasis on the vertical at work here; the lute in the foreground is directly vertical, with the line created by the neck traveling most f the way from the bottom to the top of the painting. The tree the man is leaning against, the tree behind that, and also a vertically jutting rock just beneath the tower of the distant building and a towering cloud just off the lute's neck all reinforce this sense of vertical. Tone and line contribute greatly to the two most prominent principles of design at work in the Greek Lovers. Tone produces many instances of harmony, and several of disharmony. The female figure is generally harmonious with her surroundings; her light top flows into the lighter sky to her right (viewer's left), while her other side is slightly shadowed matching the darker value of the sky above it. The man, in contrast to this, is more our of harmony with his immediate environment; though the colors of his clothes are darker then the females, the values are almost as light, yet the value of the tree he is up against is very dark. This creates a sense of disharmony...

This strange harmony/disharmony juxtaposition is mirrored in the balance of the painting. The repeated vertical lines in the trees, towers, and especially the neck of the lute all create a sense of balance and order. Careful observation reveals that the woman's torso and arm repeat this vertical line, while the man's posture creates a subtle diagonal. Just as the woman is harmonious and the man not, she is in balance and he is somehow out of it.
Gray flawlessly dovetails the elements and principles of design in the Greek Lovers to create a scene between two lovers that are somehow just our of sync; what should be a happy scene between two innocents is instead slightly disturbed by an almost indefinable quality. This quality is a result of the inconsistent balance and harmony present in the work. The painter has proved himself a master by matching the elements and principles of this painting with the subject matter to enhance the atmosphere and mood of the painting in ways that subject alone could never accomplish.