The official records of the College include registers of grants of arms, funeral certificates, the records of the heraldic visitations of the English and Welsh counties of the sixteenth and seventeenth centuries, registers of changes of name and arms by Royal Licence and deed poll, and the pedigree registers, as well as records of state ceremonials such as coronations and state funerals, and official enrolments of flags.

In addition to the official records created by the College, the archive also holds some seven thousand other manuscript volumes, and a similar number of unbound manuscripts, which have been deposited at the College or acquired by it over the centuries. These collections include working papers derived from the heraldic and genealogical practices of past heralds. Other significant holdings include the Arundel Manuscripts, primarily medieval chronicles and histories, and a large collection of manuscript pedigrees in roll form, dating from the medieval period onwards. Online exhibitions on this website give a useful overview of some of the College's holdings. The College maintains a large library of printed books.

The Records and Collections of the College of Arms, by Sir Anthony Richard Wagner (1952), gives an excellent account of the history and extent of the College archives.

A Catalogue of Manuscripts in the College of Arms Catalogue Collections volume 1 (1988), is a detailed catalogue of a small but significant part of the records and collections, including the 260 volume manuscript collection of Augustine Vincent (d.1626), Windsor Herald, and the Tudor manuscripts with the pressmarks L and M.

A Catalogue of Manuscripts in the College of Arms Catalogue Records volume 1:  Record Manuscripts of the Tudor Visitations (2023), is a detailed catalogue and index to this key series of official record manuscripts, created by the heralds in the sixteenth century. More information about the volume can be seen here. The preparation and publication of this work was kindly supported by the Marc Fitch Fund, the College of Arms Foundation, and the College of Arms Trust.