Nanoparticle–polymer composites hold promise in enabling material functionalities that are difficult to achieve otherwise, yet are hampered to date by the scarce control and tunability of the nanoparticle collective properties on the polymer surface, especially for polymer foams featuring a complex three-dimensional pore network. Here we report on the controlled and conformal in situ coating of polydimethylsiloxane (PDMS) foams with silver nanoparticles (AgNPs) with surface coverage finely tunable over a large range, from 0 to 75%, via the one-step room temperature reduction of AgF directly on the PDMS surface. This enables the design of AgNP electrical networks on the PDMS foam surface with piezo-resistive properties tunable up to a factor of 1000. We leveraged the control of the piezoresistive properties of the AgNP electrical network formed on PDMS foams to fabricate flexible and wearable pressure sensors with sensitivity of 0.41 kPa⁻¹, an operation range >120 kPa, and a detection limit of 25 Pa. As a proof-of-concept application in wearable biomedical electronics, we successfully used the sensors to monitor the real-time radial artery pulse wave on the human wrist of a young male with high resolution.