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The Correspondence series is the largest portion of the collection and dates from 1851 to 1916. The series pertains to all phases of Angell's career, university, diplomatic, and personal. Angell corresponded with a wide range of educators, diplomats, and politicians. Two folders of note, titled "Miscellaneous" and "Regarding death of Sarah Angell" contain letters to James from local organizations and university departments offering their condolences for the passing of his wife. These folders also contain a number of obituaries from Michigan and Rhode Island newspapers describing some of Sarah's Angell's major accomplishments.

The series also contains a card index to most of Angell's correspondence (Boxes 16-17). Appended to this finding aid is a selective name inventory to these correspondents listing dates of letters. The library also has an extensive (six volume), though incomplete, calendar to the Angell Correspondence series. This calendar consists of fairly detailed summarizations of the individual letters in the collection. The researcher should also note that the correspondence is primarily incoming only with very few copies of Angell's responses.

The National Archives in Washington D.C. hold Angell's microfilmed correspondence written while serving in China.