Mechanical performance of nanoparticle-based thin films depends on the method of fabrication and the properties of the underlying substrate. This study presents experimental results of electromechanical response of micrometer-thick dip-coated silver nanoparticle-based films on rough and highly compliant (Young’s modulus between 120 and 130 kPa) polydimethylsiloxane substrate having random micro-bumpy surface. The experimental results demonstrate stretchability of 13% and flexibility of 3.43% for the as-fabricated metal–polymer laminate. The entire process being amenable to mass production suggests a cost-effective and high-throughput route toward the fabrication of stretchable/flexible electronic devices and thin film sensors.