Most existing lower-limb rehabilitation robots (LLRR) for stroke and postoperative rehabilitation are bulky and prone to misalignments between robot and human joints. These drawbacks hamper LLRR application, leading to poor arthro-kinematic compatibility. To address these challenges, this paper proposes a novel robot with portability and compliance features. The developed robot consists of an underactuated mechanism and a crus linkage, respectively corresponding to the hip and knee joints. The underactuated mechanism is a new type of remote center of motion (RCM) mechanism with two sets of contractible slider cranks that can reduce the misalignments between robot and human joints. The underactuated mechanism is then optimized using the particle swarm optimization method, and the developed robot’s kinematic analysis is presented. The proposed robot can be simplified as a two-link mechanism with the ability to easily plan its trajectory using the modified Denavit–Hartenberg method. Finally, passive exercise trials demonstrate that the mismatch angles between the human and robot knee joints are less than 2.1% of the range of motion, confirming the feasibility and effectiveness of the proposed robot.