Smart sensors with self-healing capabilities have recently aroused increasing interest in applications in soft electronics. However, challenges remain in balancing the sensors' self-healing and compatibility between their sensing and substrate layers. This study evaluated several self-healing polymer substrates and graphene ink-based strain-sensing coatings. The optimum electrochemically exfoliated graphene (e-graphene)/silver nanoparticle-coated tannic acid (TA)/superabsorbent polymer/graphene oxide (GO) blended poly(vinyl alcohol) polymer composites exhibited improvements of 47.1 and 39.2%, respectively, for the healing efficiency in a substrate crack area and in the graphene-based sensing layer due to conductive layer adhesion. While TA was found to improve healing efficiency on the coating surface by forming hydrogen bonds between the sensing and polymer layers, GO healed the polymer surface due to its ability to form bonds in the polymer matrix. The superabsorbent polymer was found to absorb excess water in e-graphene dispersion due to its host-guest interaction, while also reducing the coating thickness.