We demonstrate high strain sensitivity property of gold nanoparticle (Au-NP) thin films fabricated on flexible polydimethylsiloxane (PDMS) substrates. This behavior is attributed to quantum tunneling effect that is highly dependent on nanoparticle separation. Au-NPs were synthesized in water by nanosecond laser ablation method. The clean surface providing high tunneling decay constant, size of the Au-NPs and Au-NPs aggregate clusters offer advantages for high sensitivity strain sensor. We prepared Au-NPs films on flexible PDMS substrate by using hands-on drop-cast method. To obtain high gauge factor (g factor), we investigated the nanoparticles concentration on the substrate. Laser-generated Au-NPs films demonstrated g factor of ∼300 for higher than 0.22% strain and ∼80 for the strain lower than 0.22% strain, which is favorably comparable to reported sensitivities for strain sensors based on Au-NPs. Mechanical characterizations for the prolonged working durations suggest long term stability of the strain sensors. We discuss several models describing conductance of films in low and high strain regimes.