The mechanical flexibility and structural softness of ultrathin devices based on organic thin films and low-dimensional nanomaterials have enabled a wide range of applications including flexible display, artificial skin, and health monitoring devices. However, both living systems and inanimate systems that are encountered in daily lives are all 3D. It is therefore desirable to either create freestanding electronics in a 3D form or to incorporate electronics onto 3D objects. Here, a technique is reported to utilize shape-memory polymers together with carbon nanotube flexible electronics to achieve this goal. Temperature-assisted shape control of these freestanding electronics in a programmable manner is demonstrated, with theoretical analysis for understanding the shape evolution. The shape control process can be executed with prepatterned heaters, desirable for 3D shape formation in an enclosed environment. The incorporation of carbon nanotube transistors, gas sensors, temperature sensors, and memory devices that are capable of self-wrapping onto any irregular shaped-objects without degradations in device performance is demonstrated.