Cárcano was again elected to Congress in 1910. He served as President of the Constitutional Convention of the Province of Córdoba in 1912, and briefly as Federal Receiver of San Juan Province in 1913. He was then elected Governor of Córdoba, and took office on May 17. His administration, which lasted until 1916, promoted agricultural mechanization and improved the provincial road network. He continued to write, publishing among others "La misión Mitre en el Brasil" (1913), "De Caseros al 11 de Septiembre" (1919), "Del sitio de Buenos Aires al Campo de Cepeda" (1921), and "Juan Facundo Quiroga", for which he won a National Literary Prize in 1931. Cárcano returned as Dean of the University of Buenos Aires School of Agronomy and Veterinary Medicine from 1921 to 1924, and twice served as President of the National Academy of History.