Understanding individual differences in attitudes towards Artificial Intelligence (AI) is of importance, among others in system development. Against this background, we sought to investigate associations between personality and attitudes towards AI. Relations were investigated in samples from two countries—Germany and China—to find potentially replicable, cross-culturally applicable associations. In German (N = 367, n = 137 men) and Chinese (N = 879; n = 220 men) online surveys, participants completed items on sociodemographic variables, the Attitudes Towards Artificial Intelligence (ATAI) scale, and the Big Five Inventory. Correlational analysis revealed among others significant positive associations between Neuroticism and fear of AI in both samples, with similar effect sizes. In addition to a significant association of acceptance of AI with gender, regression analyses revealed a small but significant positive association between Neuroticism and fear of AI in the German sample. In the Chinese sample, regression analyses showed positive associations of acceptance of AI with age, Openness, and Agreeableness. Fear of AI was only significantly negatively related to Agreeableness in the Chinese sample. The association of fear of AI with Neuroticism just failed to be significant in the regression model in the Chinese sample. These results reveal important insights into associations between certain personality traits and attitudes towards AI. However, given mostly small effect sizes of relations between personality and attitudes towards AI, other factors aside from personality traits seem to be of relevance to explain variance in individuals’ attitudes towards AI, as well.