Hume’s doctrine of morals is an integral part of his science of man. Both local and foreign scholars used to see it as the corresponding part between epistemology and psychology, which caused some serious misunderstanding and ignored the proper study of An Enquiry Concerning the Principles of Morals, which is the re-write of “Of Morals” in A Treatise of Human Nature. Via a comparative study of the two books, this paper contends that Hume denied the freedom of will and broke the traditional categorization of human capabilities. His doctrine of morals is a part of psychology. Based on such a thesis, this paper compares and analyzes the thoughts and views of the two books; it also points out many important developments of A Treatise of Human Nature in An Enquiry Concerning the Principles of Morals and shows the topics and clues in the latter book about how Hume strove to systemize his doctrine of morals.