Laboulaye was received at the bar in 1842, and was chosen professor of comparative law at the Collège de France in 1849. Following the Paris Commune of 1870, he was elected to the national assembly, representing the département of the Seine. As secretary of the committee of thirty on the constitution he was effective in combatting the Monarchists in establishing the Third Republic. 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. Laboulaye was also chairman of the French Anti-Slavery Society.
Laboulaye wrote poetry in his spare time. One of his poems, "L'Oiseau bleu" was set by Victor Massé.
Nevertheless, he is most remembered as the intellectual creator of the Statue of Liberty.
Always a careful observer of the politics of the United States, and an admirer of its constitution, he wrote a three-volume work on the political history of the United States, and published it in Paris during the height of the politically repressed Second Empire. and during the Civil War was a zealous advocate of the Union cause, publishing histories of the cultural connections of the two nations, while the United States was in the throes of its Civil War (1862 and 1863). At the war's conclusion, in 1865 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. The sculptor Frederic-Auguste Bartholdi, one of Laboulaye's friends, turned the idea into reality.