He studied Teaching in Santiago and founded a Primary School in his native town. He also worked as a teacher at other schools in Lugo and Ourense. In Ourense he married Elisa Pavón, worked as sub-editor of the newspaper Diario de Orense and collaborated in La Zarpa and Galicia. He also collaborated in other newspapers such as El Norte de Galicia, Vida Gallega, El Compostelano, El Correo Gallego and La Noche.He was a member of the Galician Academy and the Seminary of Galician Studies.
Couceiro Freijomil made a great bibliographical production and published works such as La aceptación del dolor (Lugo, 1914), Ortografía gallega. Bases para su unificación (Ourense, 1929), La bandera de Galicia (Ourense, 1929), Los factores del desenvolvimiento humano (Ourense, 1934), El idioma gallego, Historia, Gramática, Literatura (Barcelona, 1935), Los niños anormales y su educación especial (Ourense, 1936), Historia de Pontedeume y su comarca (Santiago, 1944), Programa escolar (Santiago, 1955).He also wrote two books that were left unpublished: Catálogo de impresos compostelanos del XVII al XIX and Cousiñas.