Completely automated public Turing test to tell humans apart (CAPTCHA) is an effective mechanism to protect websites and online applications from malicious bots programs. Image-based CAPTCHA is one of the most widely used schemes. However, deep learning techniques have significantly weakened the security of some image-based CAPTCHA schemes. Mooney images (MIs) are important research materials in the field of cognitive science. Compared to natural images, MI exhibits fewer visual cues, fragmented content, and greater ambiguity, leading to the perception of MI relying more on the iterative process between feedforward and feedback mechanisms. In this paper, we raise an intriguing question: can MIs be used to enhance the security of CAPTCHA? Before this study, we first propose a novel framework HiMI that generates the high-quality MIs from natural images and also allows flexible adjustment of the perceived difficulty. Based on MI, we design two MI-CAPTCHA schemes related to object detection and instance segmentation tasks, respectively. We experimentally demonstrate that HiMI performs better than other baseline methods in terms of both image quality and application potential in two MI-CAPTCHA schemes. Additionally, we conduct experiments to explore the solving performance of humans and CAPTCHA solvers under different parameter settings of schemes, providing valuable reference for the practical application.