This study investigates the conservation treatment options to preserve the treasured Smithsonian collection of letterpress copying books handwritten by Spencer Fullerton Baird (1823–1887), the second Secretary of the Smithsonian Institution. This study employs analytical techniques to investigate the complex nature of the materials, explores and evaluates treatment options with experimental procedures using artificially aged samples, and investigates best practices for the digitization of the materials. Technical analysis showed that iron II ion migration is a particularly severe problem in copying books and confirms a correlation between iron migration and the severity of ink corrosion. Several conservation treatments were conducted including anti-oxidant treatments, sizing, de-acidification, and paper splitting. One of the most promising treatments conducted is a non-aqueous anti-oxidant treatment using Tetrabutyl Ammonium Bromide [TBAB] in ethanol followed by non-aqueous de-acidification with magnesium oxide using the Bookkeeper spray and sizing with Klucel G in ethanol. Several imaging techniques were explored, and a simple and inexpensive set-up and procedure was found to give excellent results.