Printable robots created using origami-inspired folding processes have gained extensive attention due to their potential advantages, including low cost, rapid prototyping, lightweight, high accessibility, built-in compliance for safe interaction with humans, compact storage, etc. However, to achieve autonomy, printable robots still rely on bulky, rigid semiconductor-based electronics and their accessories (e.g., electromechanical motors), which could restrict the full potential promised by origami-inspired printable manufacturing. Here, I introduce an integrated folding-based process to create autonomous printable robots by embedding sensing, control, and actuation into compliant materials without requiring semiconductor-based electronics. By combining flexible bistable mechanisms and conductive thermal artificial muscles, we realize various autonomous behaviors. These include self-sustained locomotion and sequencing, information processing, logic and computing, and human/environment-machine interactions without the need of semiconductor-based components. Guided by theory, I have also derived simplified analytical models for the above-mentioned printable devices to enable rapid design and prototyping. Our work opens up new design space for autonomous origami machines that are low cost, lightweight, and robust to adversarial environmental factors (e.g., magnetic field and physical deformation). This thesis provides routes to achieve autonomy for printable robots through tight functional integration in compliant materials and structures.