Abstract Graphene composites possess great application potential in various fields including flexible electrodes, wearable sensors and biomedical devices owing to their excellent mechanical and electrical properties. However, it remains challenging to fabricate graphene composites-based devices with high consistency due to the gradual aggression effect of graphene during fabrication process. Herein, we propose a method for one-step fabricating graphene/polymer composite-based devices from graphite/polymer solution by using electrohydrodynamic (EHD) printing with the Weissenberg effect (EPWE). Taylor–Couette flows with high shearing speed were generated to exfoliate high-quality graphene with a rotating steel microneedle coaxially set in a spinneret tube. The effects of the rotating speed of the needle, spinneret size and precursor ingredients on the graphene concentration were discussed. As a proof of concept, EPWE was used to successfully fabricate graphene/polycaprolactone (PCL) bio-scaffolds with good biocompatibility and graphene/thermoplastic polyurethane strain sensor for detecting human motions with a maximum gauge factor more than 2400 from 40% to 50% strain. As such, this method sheds a new light on one-step in situ fabrication of graphene/polymer composite-based devices from graphite solution with low cost.