Written by Graham Gouldman, who later formed the band 10cc. Gouldman was a prolific songwriter who also came up with songs for The Hollies, Cher, The Shadows, and Herman's Hermits. For The Yardbirds, he provided three of their hits, also composing "Evil Hearted You" and "For Your Love." Yardbirds drummer Jim McCarty said: "'Heart Full of Soul,' which was very moody, gave us the ability to play the riff in sort of an Eastern way, give it an Oriental touch. Another very good song."
This was the Yardbirds' first single after Jeff Beck replaced Eric Clapton as lead guitarist. Eric Clapton left the Yardbirds in March 1965 because of a perceived shift in musical direction. Inspired in part by Jeff Beck, who replaced Clapton, the group began to experiment with different musical styles. Beck had more varied influences and used electronically enhanced guitar effects, such as fuzz and feedback, which he brought to the group's sound.
At the time, popular music at large was seen as becoming more experimental. Gouldman's arrangement was perceived as creating an exotic sound. Yardbirds' drummer Jim McCarty explained that "the riff on the [Gouldman's] demo suggested a sitar" and that the group's manager, Giorgio Gomelsky, hired a sitar and a tabla player for a recording session. The Yardbirds' first attempt to record "Heart Full of Soul" was on 13 April 1965 at Advision Studios in London. The session began with the sitar player playing the distinctive instrumental hook or riff. However, he was unfamiliar with the type of rock sound the group was trying to achieve – "It just didn't have any groove to it", Beck felt. McCarty added: "It was fine in principle, but while the tablas sounded OK, the sitar just wasn't up front enough. It just didn't cut through." Beck developed a riff on guitar to replace the sitar line. He elaborated in an interview:
"The sitar player couldn't get the 4/4 time signature right; it was a hopeless waste of time. So I said, 'Look, is this the figure?' I had the fuzz machine, a Toneblender [sic], going. We did one take, it sounded outrageous. So they kept the tabla player, who could just about make it work. They rushed that out, and the rest was a rollercoaster ride."
According to McCarty, Beck developed the riff after borrowing Page's prototype fuzz box, designed for him by Roger Mayer (Jimmy Page, who later joined the Yardbirds, was working in an adjacent studio and attended the session). When he played the lick for the band, they felt that it was a perfect fit: "this great sounding riff emerged ... I mean Beck just nailed it", rhythm guitarist Chris Dreja recalled. The group returned to Advision on 20 April to complete the song. Beck was able to achieve the sitar-like hook by bending the higher notes on his guitar in an Eastern-sounding scale while also using his own Tone Bender unit to get the distinctive tone. While simultaneously sounding the open D string, he also added a droning quality reminiscent of the sitar's sympathetic strings.
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