Parts 1 and 2 are intended as a continuation of Francis Godwin's A Catalogue of the Bishops of England published in several editions between 1601 and 1621, and are entitled, "A Collection of all Archbishops and Bishops of the Realm of England, since An[no] D[omi]ni MDCXVI unto An[no] D[omi]ni 1660." Part 1 explains what Smith intends to do and why he feels it to be necessary. Part 2, the actual collection, begins with the Archdiocese of Canterbury and its Bishoprics followed by that of York and its Bishoprics. Each entry may include: speeches, letters, an epitaph, a bibliography, a coat-of-arms, an engraved portrait, and Latin verses. These verses are taken primarily from collections of poems written for important occasions such as, the death of Prince Henry, the betrothal of Princess Elizabeth to the elector Palatine, the death of Sir Thomas Bodley, the expedition of James I to Scotland in 1617 and others, and published by the universities of Oxford and Cambridge. The sources for his information are provided and in many cases commentary on their accuracy as well. (See Bibliography). In cases where an entry for a bishop contains a 'see also' note, there is always a short entry for that See. The numbers at the head of most entries continue Godwin's numeration. It is clear from the many revisions, including crossed out sections, corrections added on pasted slips, and additions that contradict earlier statements that the work was written over a prolonged period of time probably beginning during the Civil War and continuing until at least 1665. This is unlikely to have been a final version.

Part 3 is essentially a listing of all the Archbishops and Bishops of England and Wales from the earliest times to about 1646. It gives the history of the Archbishoprics of Canterbury and York, each followed by a chronological list of the Bishops of each diocese with an opening paragraph on the origins of each. This is followed by A catalogue of the ancient Archbishoprics and Bishoprics of England now either extinct or converted into other Dioceses with the times of their first foundations and extinctions, as likewise the names of the proper Sees which belonged to them, and also the names of the modern dioceses whereunto they are reduced. There follows A discourse of the Bishops of the Isle of Man, styled in Latin Episcopi Sodorenses which discusses at some length the island's history, ending with extracts from several authors. For these Smith has often included information on the title, folio and page number. This work was probably completed about 1660.

Part 4 contains a single folio sized leaf with drawings of the Coats of Arms of each Archbishopric and Bishopric.