Graphene-based composites have received attention as part of the drive towards next-generation electronic and energy-storage technologies. However, current graphene synthesis methods are limited by complex, time-consuming, toxic, costly, and/or often low-yield procedures. The synthesis of a novel stretchable graphene-polyurethane-poly(3,4-ethylenedioxythiophene):polystyrene sulfonate ink aimed at printing wearable electronics is reported. The procedure is based on low-cost high-yield production of high-performance graphene ink produced by laser induction of polyimide film followed by harvesting the graphene. Screen printing is used to fabricate flexible and intrinsically stretchable micro-supercapacitors (S-MSCs) printed on different substrates. The resulting graphene-based printed S-MSCs display a remarkably high capacitive performance and attractive mechanical resiliency. High specific areal capacitance, above 23 mF cm−2, is achieved, which is the highest areal capacitance reported for highly stretchable, printed graphene supercapacitors. A repeated (200 cycles) stretchability beyond 100% is obtained while maintaining more than 85% of the S-MSCs' original capacitance. This unique and highly scalable graphene ink synthesis method holds considerable promise for application in low-cost graphene-based chemical formulation, especially in the field of printed and wearable electronics toward multifunctional, energy-storage systems capable of withstanding severe mechanical deformation while maintaining their optimal electrochemical performance.