Syntactic foam made from hollow glass microspheres (HGM) in an epoxy matrix has proven to be a good material with a strong structural strength. Understanding filler particle size variation is important in composite material formation, especially in syntactic foam, because of its numerous applications such as aerospace, marine, and structural purposes. In this present work, the effects of particle variation in different sizes (20–24 µm, 25–44 µm, 45–49 µm, and 50–60 µm) on the mechanical properties of the syntactic foam composites with a focus on flexural strength, modulus, and fracture surfaces are investigated. The particle sizes are varied into five volume fractions (5, 10, 15, 20, and 25 vol%). The results show that the highest flexural strength is 89 MPa at a 5 vol% fraction of 50–60 µm particle size variation with a 69% increase over the neat epoxy. This implies that the incorporation of HGM filler volume fraction and size variation has a strong effect on the flexural strength and bending modulus of syntactic foam. The highest particle size distribution is 31.02 at 25–44 µm. The storage modulus E’ increased at 30 °C, 50 °C, and 60 °C by 3.2%, 47%, and 96%, respectively. The effects of wall thickness and aspect ratio on the size of the microstructure, the fracture surfaces, and the viscoelastic properties are determined and reported accordingly.