Éamon was a founder member of Ceoltóirí Chualann, the famous folk-orchestra created by the composer Seán Ó Riada, in which Éamon played the button-accordian. Many of Ó Riada's traditional musicians were later to form the basis for the now famous traditional group The Chieftains.

When Seán Ó Riada died in 1972, Éamon de Buitléar formed his own non-professional traditional music group, Ceoltóirí Laighean. The group played on TV and radio and travelled to Continental Europe. Two commercial discs were recorded under the Gael-Linn label and some of those early recordings are being re-issued by Gael-Linn.