This paper presents abundant empirical evidence to support the view that Santiago Ramón y Cajal was a pioneer of the emerging Psychology of Science discipline. Narrative analysis of his autobiography (Recollections of my Life) and some of his unspecialized works (Advice for a Young Investigator, The World from an Eighty-Year-Old’s Point of View, and Café Chats) revealed that the Spanish histologist’s interest in the psychology of scientists was part and parcel of a high-level, intellectual self-regulation strategy he applied on his path to success. This research led him to document various psychological conclusions about scientists in writing, so as to encourage, guide, and facilitate the work of junior researchers. Current knowledge of the Psychology of Science has confirmed many of the Nobel laureate’s observations about psychosocial aspects of scientists, scientific reasoning, and creativity.