One of higher education institutions’ many goals is the development of students’ entrepreneurial intentions with the aim of encouraging entrepreneurship. Students’ entrepreneurial intentions lead towards their entrepreneurial behavior, and starting one’ company is merely one way of securing employment for students during constant and unpredictable professional challenges of the 21st century. With the aim of an effortless adjustment to both their private and professional surroundings, students should develop their career adaptability as it entails readiness and resources for successfully facing professional tasks and unexpected challenges, and should learn how to regulate and control their emotions. Emotions in business have a significant role as they affect one’s creativity, inductive and deductive reasoning, thought processes, and behavior, which is why emotional regulation and control has become a necessity. Previous research shows a direct influence of emotional intelligence on managerial and entrepreneurial skills acquisition. Thus, the question of how emotions affect not only people’s efficiency at work, their entrepreneurial judgment and behavior, but also their career adaptability has become the focus of most recent research. The main goal of this doctoral research is to explore the role of emotional regulation and control in the relationship between students’ career adaptability and entrepreneurial intentions. The purpose of this research is to use the theory of planned behavior, the theory of career construction and the model of emotional intelligence to explain the theoretical background of the constructs. The empirical contribution of this doctoral research is evidenced by the verification of connections and the explanation of interrelationships between career adaptability, emotional regulation and control, and entrepreneurial intentions. Since the role of emotional regulation and control on students’ entrepreneurial intentions has, thus far, not been investigated in Croatia, the primary research is conducted on the sample of students from the Faculty of Economics in Osijek. The data analyses consist of quantitative univariate, bivariate, and multivariate statistical research methods. When controlling for the effects of age, gender and family company, the primary research results indicate the importance of career adaptability and emotional regulation and control in predicting students’ entrepreneurial intentions. In addition, emotional regulation and control is proven to be a partial mediator of the relationship between career adaptability and entrepreneurial intentions. The obtained research results may be useful to education professionals and career counselors for raising awareness of the importance of developing students’ career adaptability and emotional regulation and control for setting their entrepreneurial intentions.