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Bartholdi and Laboulaye considered how best to express the idea of American liberty. In early American history, two female figures were frequently used as cultural symbols of the nation. One, Columbia, was seen as an embodiment of the United States in the manner that Britannia was identified with the United Kingdom and Marianne came to represent France. Columbia had supplanted the earlier figure of an Indian princess, which had come to be regarded as uncivilized and derogatory toward Americans. The other significant female icon in American culture was a representation of Liberty, derived from Libertas, the goddess of freedom widely worshipped in ancient Rome, especially among emancipated slaves. A Liberty figure adorned most American coins of the time, and representations of Liberty appeared in popular and civic art, including Thomas Crawford's Statue of Freedom (1863) atop the dome of the United States Capitol Building.

Artists of the 18th and 19th centuries striving to evoke republican ideals commonly used representations of Liberty. A figure of Liberty was also depicted on the Great Seal of France. However, Bartholdi and Laboulaye avoided an image of revolutionary liberty such as that depicted in Eugène Delacroix's famed Liberty Leading the People (1830). In this painting, which commemorates France's Revolution of 1830, a half-clothed Liberty leads an armed mob over the bodies of the fallen. Laboulaye had no sympathy for revolution, and so Bartholdi's figure would be fully dressed in flowing robes. Instead of the impression of violence in the Delacroix work, Bartholdi wished to give the statue a peaceful appearance and chose a torch, representing progress, for the figure to hold.

Crawford's statue was designed in the early 1850s. It was originally to be crowned with a pileus, the cap given to emancipated slaves in ancient Rome. Secretary of War Jefferson Davis, a Southerner who would later serve as president of the Confederate States of America, was concerned that the pileus would be taken as an abolitionist symbol. He ordered that it be changed to a helmet. Delacroix's figure wears a pileus, and Bartholdi at first considered placing one on his figure as well. Instead, he used a diadem, or crown, to top its head. In so doing, he avoided a reference to Marianne, who invariably wears a pileus. The seven rays form a halo or aureole. They evoke the sun, the seven seas, and the seven continents, and represent another means, besides the torch, whereby Liberty enlightens the world.

Bartholdi's early models were all similar in concept: a female figure in neoclassical style representing liberty, wearing a stola and pella (gown and cloak, common in depictions of Roman goddesses) and holding a torch aloft. The face was modeled after that of Charlotte Beysser Bartholdi, the sculptor's mother. He designed the figure with a strong, uncomplicated silhouette, which would be set off well by its dramatic harbor placement and allow passengers on vessels entering New York Bay to experience a changing perspective on the statue as they proceeded toward Manhattan. He gave it bold classical contours and applied simplified modeling, reflecting the huge scale of the project and its solemn purpose. Bartholdi wrote of his technique:

Thomas Crawford's Statue of Freedom

The surfaces should be broad and simple, defined by a bold and clear design, accentuated in the important places. The enlargement of the details or their multiplicity is to be feared. By exaggerating the forms, in order to render them more clearly visible, or by enriching them with details, we would destroy the proportion of the work. Finally, the model, like the design, should have a summarized character, such as one would give to a rapid sketch. Only it is necessary that this character should be the product of volition and study, and that the artist, concentrating his knowledge, should find the form and the line in its greatest simplicity.

Bartholdi made alterations in the design as the project evolved. Bartholdi considered having Liberty hold a broken chain, but decided this would be too divisive in the days after the Civil War. The erected statue does rise over a broken chain, half-hidden by her robes and difficult to see from the ground. Bartholdi was initially uncertain of what to place in Liberty's left hand; he settled on a tabula ansata, a keystone-shaped tablet used to evoke the concept of law. Though Bartholdi greatly admired the United States Constitution, he chose to inscribe "JULY IV MDCCLXXVI" on the tablet, thus associating the date of the country's Declaration of Independence with the concept of liberty.

Consultations with the metalwork foundry Gaget, Gauthier & Co. led Bartholdi to conclude that the skin should be made of copper sheets, beaten to shape by the repoussé method. An advantage of this choice was that the entire statue would be light for its volume—the copper need be only .094 inches (2.4 mm) thick. He decided on a height of 151 feet (46 m) for the statue, double that of Italy's Colosso di San Carlo Borromeo and the German statue of Arminius, both made with the same method. Bartholdi interested a former teacher of his, architect Eugène Viollet-le-Duc, in the project. Viollet-le-Duc planned to construct a brick pier within the statue, to which the skin would be anchored.