Upon its release, "There Must Be an Angel (Playing with My Heart)" became Eurythmics' first (and to date only) number-one single in the United Kingdom, reaching number one on 27 July 1985 and staying there for one week, whilst also topping the charts in Finland, Ireland and Norway.

The song also reached the top 10 in Australia, Austria, Belgium, France, Germany, the Netherlands, New Zealand and Sweden, while peaking at number 22 on the US Billboard Hot 100.

Cash Box said that the "Annie Lennox harmonies, slick Dave Stewart production work and Stevie Wonder's incredible harmonica" were highlights of the song.

"[2] The music video for "There Must Be an Angel (Playing with My Heart)", directed by Eddie Arno and Mark Innocenti, was shot at New Wimbledon Theatre in London in June 1985.

It portrays the times of Louis XIV of France (David A. Stewart) being entertained while watching a theatre performance of singing angels (one of which is played by Steven O'Donnell).

In mid-2001, producers Patrik Majer, Ulf Leo Sommer, and Rosenstolz member Peter Plate consulted on a contemporary version of the track, recorded by German girl band No Angels.

[53] Inspired by Tony Scott's 1986 film Top Gun, the clip features the quintet as fighter pilots of the fictional US military squadron 68 at an also-fictional airbase in Angelville, United States.

Additionally, it incorporates a 1940s World War II theme, heavily inspired by performances of Marilyn Monroe, The Andrews Sisters and others during their USO shows.