In this work, a novel platform for surface-enhanced Raman spectroscopy (SERS)-based chemical sensors utilizing three-dimensional microporous graphene foam (GF) decorated with silver nanoparticles (AgNPs) is developed and applied for methylene blue (MB) detection. The results demonstrate that silver nanoparticles significantly enhance cascaded amplification of SERS effect on multilayer graphene foam (GF). The enhancement factor of AgNPs/GF sensor is found to be four orders of magnitude larger than that of AgNPs/Si substrate. In addition, the sensitivity of the sensor could be tuned by controlling the size of silver nanoparticles. The highest SERS enhancement factor of ∼ 5 × 10(4) is achieved at the optimal nanoparticle size of 50 nm. Moreover, the sensor is capable of detecting MB over broad concentration ranges from 1 nM to 100 μM. Therefore, AgNPs/GF is a highly promising SERS substrate for detection of chemical substances with ultra-low concentrations.