Abstract: The present invention relates to a process for preparing a polyurethane composite material, comprising steps of: I) preparing a premolded polyurethane molding body, wherein the premolded polyurethane molding body is prepared from a polyurethane composition under a condition that isocyanate groups and isocyanate-reactive groups comprised in the polyurethane composition undergo an addition reaction; II) curing the premolded polyurethane molding body to prepare the polyurethane composite material, wherein the premolded polyurethane molding body cures by the radical polymerization of active olefinic bonds. The process of the present application has a lower TVOC value and better processability.