The 19 Norwegian Folksongs, Op. 66 are remarkable pieces, as Grieg himself knew. He wrote to the Dutch composer, Julius Röntgen, of having "put some hair-raising chromatic chords on paper. The excuse is that they originated not on the piano but in my mind. If one has the Vøringfoss beneath one's feet, one feels them more independent and daring than down in the valley."

Indeed, the harmonies that Grieg employs in Op. 66 are even more strongly chromatic in flavor than those in his previous set of Norwegian Folk Tunes Op. 17, often to the extent that some of the chords and progressions would undoubtedly grate on the ear of the folk song purist. Nevertheless, given the fundamentally banal character of the original songs, some commentators have conceded that Grieg's chromatic treatment tends to enhance their haunting charm.

Among the 19 tunes are several longer pieces, as well as three derived from "cattle calls," the brief snatches of melody that were originally sounded to call cattle back to the fold, and have a kind of charming, far-away character. Among the most attractive is "I Ola-Dalom, i Ola-Kjönn" (In Ola Dale), No. 14, which Delius later used as the source of the theme for "On hearing the first cuckoo in spring." The melody is treated strophically, and an interlude between each verse determines the style of accompaniment for the next.

Another remarkable piece is No. 18, "Jeg går i tusind Tanker" (In deepest thought I wander), the most purely pianistic and—at four minutes long—the longest of the collection. Based on a flowing 16-bar tune, the piece is marked andante religioso, and is characterized by the same fervor and sincerity of Grieg's last opus (74), the "Four Psalms" for unaccompanied choir.

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