Piezoresistive properties play a vital role in the development of sensor for structural health monitoring (SHM) applications. Novel stable crack initiation method (SCIM) is established to improve the gauge factor (GF) with maximum achievable working strain region for PI tape enabled buckypaper hybrid sensors. Cracks are generated by applying strain rate-controlled tension force using dynamic mechanical analyzer (DMA). The sensor has been cycled in tension to characterize GF with crack opening. It is determined experimentally that GF increases with increasing crack opening and crack becomes unstable when opening increases above 8 µm. Tremendous improvement in GF has been observed which improved from single-digit to several hundreds. The highest GF obtained so far is ~255, showing 75 times improvement compared with the ones without the SCIM implementation. The crack initiation strain (CIS) is characterized by sonication and centrifugation time. It is determined experimentally that the maximum CIS of 3.5% can be achieved with sonication time of 40 min and increasing centrifuge time has an in-significantly dropping effect on CIS. Excellent stability/reproducibility has been proved/demonstrated on SCIM implemented sensors through a rigorous 12,500 tensile cycle test on DMA. The performance of sensor is practically demonstrated in tension and bending on glass fiber reinforced polymer (GFRP) structures.