It is well known that supplementary cementitious materials (SCMs) have obvious effects on the properties of concrete. In order to understand the relationship between cementitious materials and properties of ultrahigh strength concrete (UHSC), the cementitious compositions of UHSC were designed by the simple-centroid design method. The effects of cementitious compositions on the properties of UHSC were investigated. It was found that the incorporation of silica fume (SF) improved the flowability and strength of UHSC, but it decreased the time of acceleration period, calcium hydroxide (CH) content, and porosity of UHSC at a certain content. The incorporation of fly ash (FA) increased the flowability, time of acceleration period, and porosity of UHSC, but it decreased the strength and CH content of UHSC. The relationships between cement, silica fume, and fly ash and the properties of UHSC were calculated based on the simple-centroid design method.