She led a group studying the Bible at Abbey Road Congregational chapel in the British seaside town of Torquay where she was caring for her brother.

[5] After a brief sojourn in England during the first months of 1855,[4] the couple set out for Petrópolis, Brazil in April where they were welcomed into the Catholic country by their neighbor Brazilian emperor Pedro II.

The country also provided a welcoming religious climate that allowed Kalley's Portuguese-speaking followers from Madeira to join them.

By 1856 they established a Portuguese evangelical church, which was formally organized on July 11, 1858 as Igreja Evangélica Fluminense [pt].

[7] Sarah advocated the power of faith through song, and the couple created a hymnal in the Portuguese language.

[4] The songs had been checked by a native Portuguese speaker after they were written, but some words like "white as snow" can still reflect the author's background.

[10] Sarah authored The Life of John Bunyan, and was the co-Portuguese language translator of his novel The Holy War.