Events around the world this year celebrate the bicentenary of the birth of Charles Darwin (1809–1882) and the sesquicentenary of publication of his most important work, The Origin of Species (Darwin 1859). The associated plethora of books and papers now appearing to commemorate Darwin's work continue the traditional emphasis on his zoological and geological contributions. There has been some recent attention directed towards Darwin's relatively unsung but significant accomplishments as a botanist. Here, we bring together a review of Darwin's botanical discoveries and experiments and relevant aspects of his geological investigations, with a focus on the Southern Hemisphere. This is a relatively unexplored aspect of Darwin's contributions that yields some new insights meriting future research.