Objective: The purpose of this study was to investigate the effects of Tai Chi (TC) on arterial stiffness, physical function of lower-limb, and cognitive ability in adults aged over 60. Methods: This study was a prospective and randomized 12-week intervention trial with three repeated measurements (baseline, 6, and 12 weeks). Sixty healthy adults who met the inclusion criteria were randomly allocated into three training conditions (TC-24, TC-42, and TC-56) matched by gender, with 20 participants (10 males, 10 females) in each of the three groups. We measured the following health outcomes, including markers of atherosclerosis, physical function (leg power, and static and dynamic balance) of lower-limb, and cognitive ability. Results: When all three TC groups (p < 0.05) have showed significant improvements on these outcomes but overall cognitive ability at 6 or 12 weeks training period, TC-56 appears to have superior effects on arterial stiffness and static/dynamic balance in the present study. Conclusions: Study results of the present study add to growing body of evidence regarding therapeutic TC for health promotion and disease prevention in aging population. Future studies should further determine whether TC-42 and TC-56 are beneficial for other non-Chinese populations, with rigorous research design and follow-up assessment.