The materials in the Raymond Smyke collection consist of personal papers, correspondence, publications, photographs, newspapers and reports accumulated during his time as the World Organization of the Teaching Profession Secretariat, WCOTP Special Assistant for Africa, and in the case of his personal correspondence, some time after. The collection has twelve series:

1. WCOTP
2. WCOTP Conferences
3. WCOTP All American Conference on Health, Physical Education and Recreation
4. WCOTP Role of Women in African Teaching Association Meeting
5. NTAL
6. NTAL Convention
7. Correspondence/Personal Papers
8. Reports
9. Other Organizations
10. Other Meetings
11. Newspapers/Clippings/Writings
12. Miscellaneous

The WCOTP series contains correspondence between Smyke and a number of individuals, mostly regarding subjects and activities within the WCOTP or NTAL. This series also contains reports, pamphlets, programs, lists of African memberships, curriculum vitas, and photos.

The WCOTP Conferences series is divided by continent and contains correspondence about each conference as well as programs, notes, reports, evaluations, schedules, committees, attendance lists, applications, minutes, curriculum vitas, and budgets. This series contains documents in both English and French.

The WCOTP All African Conference on Health, Physical Education and Recreation series contains correspondence dealing most with invitations, attendance, and general conference planning. The rest of the series contains background information, articles regarding the conference, announcements, supply invoices, programs and indexes. This series contains documents in both English and French.

The WCOTP Role of Women in African Teaching Association Meeting is made up of correspondence, background information, evaluation and information sheets, questionnaires, invitations, credential forms, attendance lists, participant/guest lists, participant biographical sheets with corresponding photos, budget and supply information, travel arrangements, resolutions and recommendations, programs, schedules, speeches and selections presented at the conference, photos, newspaper articles regarding the conference, notes, reports and a newsletter published about the conference in Papua New Guinea. Also included in this series are sign up sheets for various seminars.

The NTAL series includes correspondence, accomplishments, booklets, questionnaires, a code of ethics, constitutions, resolutions, invoices, receipts, information regarding dues and expenses, drafts and final copies of the NTAL history, correspondences about and drafts of the NTAL letterhead including copies of blank letterheads, bulletins, information regarding education week including newspaper clippings and themes, programs, schedules, payment drafts, business cards, newspaper clippings, minutes, floor plans of the proposed Teacher's Association building for NTAL. Prominent names in this series include Albert Porte, William G. Carr, Florence Ricks-Bing, and WCOTP President, Motofumi Makieda. There are some documents in this series that are illegible. Documents in this series are in English, French and Japanese.

The NTAL Conventions series is divided by location in Africa or by the specific convention. Folders are organized by year starting with the oldest convention. This series contains correspondence regarding the details of these conventions as well as articles, programs, announcements, press releases, checks, receipts, account statements, attendance, and working papers. This series also contains "Educating the Child in the Rural Community" by Fay Saunders and a translation of a report written by Thure Sjödhal and Yngve Svensson.

The Correspondence/Personal Papers series is where correspondence not dealing with a specific action of an organization was placed. This sibseries also contains quite a bit of personal correspondence and papers between Smyke and several individuals before and after his retirement from WCOTP. It is divided by the name of the person that created the document or the person that the document concerns. This series contains biographical information on A. Doris Banks-Henries, Ora M. Horton, Florence Ricks-Bing and A. Timothy Summerville as well as publications by Mary Antoinette Brown, Foday J. Massaquoi, Ora M. Horton, Georgia Miller and Albert Porte. The correspondence between Smyke and Verlon Stone regarding the deposit of his papers into the Liberian Collections Project is also contained in this series along with appeals directed toward Smyke for education or employment assistance in addition to school transcripts, curriculum vitas and scholarship information.

The Reports series contains a series of transcript drafts of Glenna Ingold tapes during her three month African tour under an O.S.S.T.F. travel fellowship. Cover letters to these reports are also included. Tape one is from Ethiopia, tape two Kenya, tape three Uganda, tape four Mombasa and Zambia, tape five Lusaka, tape six Nigeria, tape seven Ghana and tape eight Sierra Leone. The NTAL reports in this series include those written by the delegate representing NTAL at the WCOTP conference in Copenhangen, the annual report of the Executive Secretary of the NTAL to the Representative Assembly in Harper City, Cape Palmas and the Report of the Executive Secretary of the NTAL May 24, 1973-May 15, 1974. The WCOTP portion of this series contains reports to the WCOTP Executive by African Groups and the report of the first WCOTP African Regional Conference. There is also a list of the Monrovia report distribution. There are two reports in this series regarding the Operations Crossroads Africa In-Service Teaching Training Project. The "Special Report on the Principal Needs of the Government of Liberia in the Field of Education with Implications for Future Planning" by the Ministry of Education and the "University of Botswana, Lesotho, and Swaziland Annual Report of the School of Education for 1967" are also included in this series.

The Other Organizations series houses documents that did not fit under the WCOTP or NTAL subject headings. These organizations are UNESCO, the United Nations and WCEA. The series contains newsletters, programs, mailing lists, agendas, reports and "Recommendations Concerning the Status of Teachers" by the UN Educational, Scientific, and Cultural Organization. Documents in this series are in both English and French.

The Other Meetings series contains documents regarding meetings that were not organized by WCOTP or NTAL. The West African Seminar on Rural Home Economics was organized by WCOTP, NTAL and SFL so papers regarding this seminar were also placed under this series. Also included in this series are the Cross-Cultural Cooperation in National Development /Upward Bound, Liberian Social Science Research and the Writer's Conference and International Textbook Project meetings. The series contains correspondence, order forms for working papers, press releases, reports, registration forms, itineraries, photos and bulletins.

The Newspapers/Clippings/Writings series is divided by individual newspaper name and includes The Liberian Age, The Listener, The Liberian Star and others. This series also contains correspondence and miscellaneous publications written by Smyke, Albert Porte, Augustine Jappah, James K. Momoh and Victoria Wreh amongst others. The epic poem "Siaka and Willy" by Askia S. Massaquoi is a part of this series.

The Miscellaneous series contains information on the International Development Association, the Liberian Studies Association as well as drafts, memos, and notes. Also included in this series are programs, a political map of Liberia, a map of Bong County, a painting of the Bong county flag, the Bong Range Project technical information booklet and the B.W.I. 1969 Review booklet and pictures.

The Publications series contains several publications by such noted Liberians as Doris Banks-Henries and Mary Antoinette Grimes-Brown as well as the Liberian Historical Society, the Ministry of Education and the University of Liberia.