The incomplete decomposition of foaming agent and tedious process during the preparation of epoxy resin composite foam (ERCF) will reduce the mechanical properties and lead to more complex production. Therefore, in this study, a new and simple negative pressure foaming method was designed innovatively to prepare ERCF under negative pressure using strong gas adsorption capacity of inorganically modified calcium silicate (MCS) particles as air carriers instead of foaming agent, and the density and expansion ratio of ERCF could be precisely controlled by adjusting the negative pressure value in a vacuum oven. The results showed that the density of ERCF could reach a very low value of 0.056 g/cm3 at 15 wt% MCS content with decreased negative pressure, but the negative pressure decreases would damage the quality of cells. At the same time, it was found that a rapid rise in the viscosity of the epoxy composite material system under negative pressure of −0.080 MPa owing to the increase in MCS content, when the MCS content was higher than 15 wt%, the MCS dispersion was reduced, leading to a decrease in the quality of the cells. In addition, the ERCF products prepared by the negative pressure foaming method in this study could be easily molded and possessed a better compressive strength among epoxy foams of similar density.