Micro/nano serpentine structures have widespread applications in flexible/stretchable electronics; however, challenges still exist for low-cost, high-efficiency and controllable manufacturing. Helix electrohydrodynamic printing (HE-printing) has been proposed here to realize controllable direct-writing of large area, highly aligned serpentine micro/nanofibers by introducing the rope coiling effect into printing process. By manipulating the flying trajectory and solidification degree of the micro/nano jet, the solidified micro/nanofiber flying in a stabilized helical manner and versatile serpentine structures deposited on a moving collector have been achieved. Systematic experiments and theoretical analysis were conducted to study the transformation behavior and the size changing rules for various deposited microstructures, and highly aligned serpentine microfibers were directly written by controlling the applied voltage, nozzle-to-collector distance and collector velocity. Furthermore, a hyper-stretchable piezoelectric device that can detect stretching, bending and pressure has been successfully fabricated using the printed serpentine micro/nanofibers, demonstrating the potential of HE-printing in stretchable electronics manufacturing.