The extensive holdings of the ABC cover Bethune's entire career. They consist of manuscript and printed materials, as well as a large variety of non-textual materials (graphic, sound, artifact). Included in the Collection are:
- Approximately 400 linear feet of papers, books, periodicals, drawings, photographs, slides, films, and audio/video tapes
- About 170 cubic feet of oversized drawings, architectural plans, models, paintings, textiles, and artifacts
- Examples of Bethune's work in many media: ink on paper, tempera, silkscreen, bronze, pewter, wood, textile, clay, and stained glass
Highlights include:
- Correspondence with Dorothy Day and the Catholic Worker community
- Correspondence with Graham Carey on art and the Catholic Art Association
- Project files from her U.S. and international church projects
- Manuscripts and published writings on liturgical and social justice issues for Catholic Art Quarterly, Liturgical Arts, Orate Fratres/Worship, Church Property Administration, etc.
- Writings and drawings for children
- Records and inventory of St. Leo Shop, her business selling liturgical items for home use
- Records of the Church Community Housing Corporation, which provided affordable housing, and of Harbor House, a new-model elderly living community, both in Newport, RI