The teaching of the phenomenon of radioactivity is considered a key ingredient in the path towards developing critical thinking skills in many secondary science education curricula. Despite being one of the basic concepts in general physics courses, the scientific teaching literature of the last 40 years reports a great deal of misconceptions and conceptual errors related to radioactivity that seemingly appear regardless of the educational level and context. This study reports the first cross-sectional diagnostic study in Spain to secondary education students and pre-service teachers. Data were collected in the year 2019 through a questionnaire adapted from a previously validated one to explore the main misconceptions, attitudes, and knowledge status on the topic on a sample of 191 secondary school students and 29 Physics-and-Chemistry trainee teachers in the Spanish region of Valencia. Open and closed questions were used to categorize the entity itself, its properties, and the main misconceptions related to radioactivity. The responses were analysed using conventional statistical methods. The results indicate an evolution from a widespread dissenting notion on the phenomenon, which is staunchly related to danger, hazard, and destruction in the lowest educational levels, towards a more rational, relative, and multidimensional perspective in the highest ones. On the other hand, the ideas, emotions, and attitudes of the inquired individuals are in good agreement with the main misconceptions reported in the literature.