Richard Smith was a collector of unusual and often macabre objects, among them death masks of hanged criminals, which he made himself, and the account of a murder trial, bound in the skin of the young man found guilty and hanged. Much of his large anatomical collection was inherited from his father, also a surgeon, and he used it for lectures at the Philiosophical and Literary Society at the Bristol Institution. Smith Junior also collected objects from around the world, including clothes and weapons from Native North America, and animal remains- often with deformities.

In 1827 the museum was institutionalised within Bristol Royal Infirmary. Smith Junior and surgeon Richard Lowe donated their prepared collections and books. It was open in the west wing of the Infirmary for additions, viewings and lectures. It displayed medical specimens, which served as a status symbol for Smith and the memory of his father. Few of the human remains are associated with names, more usually they were labelled with the surgeon who worked on or collected them.

In 1860, a purpose built museum opened, below Fripp's Chapel, part of Bristol Royal Infirmary. It was an opportunity, since Smith had died in 1843, to rearrange specimens. This museum also contained microscopes, reference books, and photography facilities.

Part of Smith's collection is now at Bristol Museums, some remained at Bristol Infirmary. Some of the human remains were buried (such as the skeleton of John Horwood in 2011, 190 years after he was executed) or destroyed. Smith's paperwork can be viewed at Bristol Archives.