A solution casting approach is used to create hollow glass microsphere (HGM)-filled epoxy–syntactic foam composites (e–SFCs) by varying the concentrations of HGM in epoxy according to different particle sizes. Density analysis is used to investigate the impact of concentration and particle size regularity on the microstructure of e-SFCs. It was observed that e–SFCs filled with an HGM of uniform particle sizes exhibit a reduction in density with increasing HGM concentration, whereas e-SFCs filled with heterogeneous sizes of HGM exhibit closeness in density values regardless of HGM concentration. The variation in e–SFC density can be related to HGM packing efficiency within e–SFCs in terms of concentration and particle size regularity. The particle size with lowest true density of 0.5529 g/cm3, experimental density of 0.949 g/cm3 and tensile strength of 55.74 MPa resulted in e-SFCs with highest specific properties of 100.81 (MPa·g/cm3), with a 35.1% increase from the lowest value of 74.64 (MPa·g/cm3) at a true density of 0.7286 g/cm3, experimental density of 0.928 g/cm3 and tensile strength of 54.38 MPa. The e–SFCs’ theoretical density values were obtained. The variance in theoretical and experimental density values provides a thorough grasp of packing efficiency and inter-particle features.