Soft materials have gained increasing prominence in science and technology over the last few decades. This shift from traditional rigid materials to soft, compliant materials have led to the emergence of a new class of devices which can interact with humans safely, as well as reduce the disparity in mechanical compliance at the interface of soft human tissue and rigid devices.<br><br>One of the largest application of soft materials has been in the field of flexible electronics, especially in wearable sensors. While wearable sensors for physical attributes such as strain, temperature, etc. have been popular, they lack applications and significance from a healthcare perspective. Point-of-care (POC) devices, on the other hand, provide exceptional healthcare value, bringing useful diagnostic tests to the bedside of the patient. POC devices, however, have been developed for only a limited number of health attributes. In this dissertation I propose and demonstrate wireless, wearable POC devices to measure and communicate the level of various analytes in and the properties of multiple biofluids: blood, urine, wound exudate, and sweat.<br><br>Along with sensors, another prominent area of soft materials application has been in actuators and robots which mimic biological systems not only in their action but also in their soft structure and actuation mechanisms. In this dissertation I develop design strategies to improve upon current soft robots by programming the storage of elastic strain energy. This strategy enables us to fabricate soft actuators capable of programmable and low energy consuming, yet high speed motion. Collectively, this dissertation demonstrates the use of soft compliant materials as the foundation for developing new sensors and actuators for human use and interaction.