The son of a goldsmith Barye started to work at 13 as an apprentice to an engraver and then for Bicunais, a goldsmith. Such apprenticeship enabled him to discover the secrets of metals, notably foundry and chiselling methods.
Barye then worked in 1816 with Bosio, a sculptor, and studied at the school of Beaux-Arts in Paris from 1818 until 1824. In 1820 he was awarded a second prize medal with a sculpture entitled "Cain cursed by God" and started to earn a living working for Fauconnier, a goldsmith for whom he produced small-size animals.
Barye however found his main source of inspiration in the gardens of the Paris Natural Museum (Jardin des Plantes) where he studied captive animals and took a keen interest in anatomy.
He faced many difficulties during his career, notably in 1848 when his patrons demanded the reimbursement of a considerable sum of money and seized all his models in return. Appointed as head of the department of plaster moulds of the Louvre Museum in 1848, Barye gave up his job two years later in favour of Nieuwekerk. He then taught drawing at the Museum of Natural History in 1854 and was awarded the medal of the Légion d'Honneur the following year. Elected at the French Academy in 1868, he sought refuge in Cherbourg during the 1870 Franco-Prussian war and returned to Paris in 1871.