The Neil C. Macdonald Papers consist primarily of materials related to his educational career. Included are his writings, some of which were composed while he was the State Superintendent of Public Instruction. Other items pertain to his time at Harvard University, his illness and death, and to other members of the Macdonald family.

125 photographs were separated and placed in the Photograph File Cabinets. Most of the photographs depict Neil Macdonald and his work in the field of education. There are also several photographs of the extended Macdonald family.