According to Ethel Bailey Higgins, former curator of botany at the San Diego Natural History Museum, Orcutt was an earnest and eager collector in all lines of natural history. He contributed many new and interesting items to the field of science. Even as a child, Charles Russell Orcutt described his early fascination with collecting: "Since my earliest remembrance I have been a collector and usually amused myself at first with collections of buttons, paper men and later with the addition of beans."

In 1875, Orcutt began a garden and by the fall, he had acquired 202 varieties of beans that he displayed at the annual county fair in Woodstock, Vermont. When he was only 13 years old, Charles Orcutt began his botanical collections by gathering all different types of wood, nuts and seeds. It seems only natural that Orcutt chose this field of work, which combined his love of nature and interest in diverse forms of natural history, with his keen interest in collecting.

Orcutt's heritage can be seen in the scientific names used for many of his discoveries, specifically for the various species of mollusks and plants he discovered in Baja California (1882-1919). During this time Baja California was a new area to be explored and C.R.Orcutt was the first botanical collector to survey the area. One discovery he made on his journeys was a 'lost' cactus of Baja California, the Pachycereus orcuttii; Orcutt cut a piece from it and let the plant grow for 20 years in his yard. A type of cactus was found in Baja California with bright yellowish spines, and was later named in honor of Orcutt, Cereus orcuttii, by Katherine Brandegee. Over the years Orcutt found 75 proposed taxa including fifteen plant species and one genus that were named in his honor. (For list, see Eponymous Species.)

The materials C.R. Orcutt collected included not only natural history materials (i.e. shells, seeds, living plants), but also natural history books, minerals, fossils, and herbarium specimens. Orcutt was a collector who wanted to share what he had found with others. He would send the specimens to an institution and would become displeased if they were not studied. From his collections, he often advertised material he found for sale. He contributed much of his collection to various museums in the United States, such as the Smithsonian Institute, Philadelphia Academy of Science, the American Museum of Natural History, as well as the San Diego Natural History Museum.