In this study, the MoS2 nanoparticles grown on crumpled 3D graphene microball (3D GM–MoS2) was synthesized using a microfluidic droplet generator with thermal evaporation-driven capillary compression and hydrothermal reaction. The morphology and size of 3D GM–MoS2 are controlled by the concentration of nano-sized graphene oxide (GO) and the flow rate of oil phase on the droplet generator. The 3D GM–MoS2 with fully sphere-shape and uniform size (~ 5 μm), and homogeneous growth of MoS2 nanoparticles could be synthesized at the flow rate of the oil phase of 60 μL/min with the optimized GO concentration of 1.0 mg/mL, and ( NH4)2MoS4 concentration of 2.0 mg/mL.