Mr. Gordon conceded he didn’t think too much of Unforgettable when he wrote it in 1951, but changed his mind when Nat “King” Cole made it a hit. Irving Gordon, composer of popular songs who was best known for the Grammy-winning Unforgettable, has died. He was 81.

Mr. Gordon, who also wrote the recently revived Prelude to a Kiss, died on Sunday in Los Angeles.

He earned the song-of-the-year Grammy in 1992 after Natalie Cole included Unforgettable in her album of duets with original recordings by her late father, Nat “King” Cole. Mr. Gordon conceded he didn’t think too much of his song when he wrote it in 1951, but quickly changed his mind when the elder Cole played it, liked it and made it one of his signature hits.

“It’s nice to have a song come out that doesn’t scream, yell and have a nervous breakdown while it talks about tenderness,” he told a New York audience when he received the Grammy. “People … want a melody. They want to be able to sing a song.”

Mr. Gordon had written Prelude to a Kiss, giving title and lyrics to a tune by Duke Ellington, while riding a New York subway in the late 1930s. Half a century later the song enjoyed renewed popularity in connection with the play and motion picture of the same title.

Especially clever with titles, Mr. Gordon also penned the song Throw Momma From the Train, which was recorded by Patti Page in 1956. In recent years, the title headed a Danny DeVito film.

Other Gordon credits include lyrics for What Will I Tell My Heart? recorded by Bing Crosby, and Me, Myself and I, recorded by Billie Holiday. Those hits won him a songwriting contract for Ellington in 1937, and his career was launched.

In the 1940s and 1950s, Mr. Gordon continued to churn out hits such as Mr. and Mississippi and What Did Della Ware.

Known for his plays on words, Mr. Gordon also wrote the classic comedy routine made famous by Abbott and Costello and known as “Who’s on First?” By 1960, tastes in popular music had veered away from rhyming lyrics set to hummable melodies.

“All of a sudden, the old-timers, there was no market for them,” he told the Los Angeles Times in 1988. “So I became a tennis pro. I have many lives.”

Mr. Gordon had spent his time in recent years writing a musical, Dr. Freud Will See You Now, which has never been performed.