Laboulaye was received at the bar in 1842, and was chosen professor of comparative law at the Collège de France in 1849.

In 1875, he was elected a life senator, and in 1876 he was appointed administrator of the Collège de France, resuming his lectures on comparative legislation in 1877.

During the American Civil War, he was a zealous advocate of the Union cause and the abolition of slavery, publishing histories of the cultural connections of the two nations.

At the war's conclusion in 1865, he became president of the French Emancipation Committee that aided newly freed slaves in the U.S.[1] The same year he had the idea of presenting a statue representing liberty as a gift to the United States, a symbol for ideas suppressed by Napoleon III.

Laboulaye also translated into French the autobiography of Benjamin Franklin and the works of Unitarian theologian William Ellery Channing.