Perhaps Nielsen's greatest piano work, the Suite, FS 91 was written in late 1920 and early 1921, in part at Nielsen's summer home on Skagen (the northernmost part of Denmark) and in part in Gothenburg, Sweden (where Nielsen guest conducted a few months out of the year). Dedicated to Artur Schnabel, it was first performed by Johanne Stockmarr, a pupil of Nielsen's who played the premieres of many of his piano works, in Copenhagen on March 14, 1921. The Suite originally carried the title "The Luciferian," Nielsen's reference being to Lucifer, the herald of the day and light-bearer of Greek mythology. But after several critics and listeners misunderstood and looked in the music for demonic elements, Nielsen dropped the title.

To help performers understand his intentions, Nielsen added some brief performance notes in the published score. He felt a "cold and brittle" tone was appropriate for the first piece, which begins innocuously but leads to considerable storminess before returning to its initial calm. The second movement glistens, emphasizing the upper end of the keyboard. "Supreme calm and strength" and "a certain brutal temper" were Nielsen's prerequisites for the powerful third piece, which features the obsessive repetition of short phrases so familiar from other of his works. After a playful interlude, requiring (according to Nielsen) a "completely cool, transparent presentation," the fifth piece is brief and enigmatic, not quite certain if its light-heartedness is genuine. The sixth and final piece is a manic eruption, wildly energetic and explosive; a lovely moment of stasis at the midpoint only emphasizes its power.

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