In order to achieve better sealing of boreholes, the performance of sealing materials is modified to improve the efficiency of coalbed methane extraction. In this paper, a new type of cement-based hole sealing material was prepared by using silicate cement (PC) and cement sulfoaluminate (SAC) as raw materials, supplemented with various additives, such as fly ash, Na 2 SO 4 , Ca(OH) 2 , and poly(vinyl alcohol) (PVA) fiber. The effects of these additives on the fluidity, setting time, and compressive strength of the PC-SAC compounded cementitious pore sealing material were investigated by orthogonal tests, and the hydration process and hydration products were analyzed by X-ray diffraction (XRD), thermogravimetry-differential thermogravimetry (TG-DTG), and scanning electron microscopy (SEM). The results show that the water−cement ratio has the most significant influence on the various properties of the material; the two additives of Na 2 SO 4 and Ca(OH) 2 play a key role in the setting time of the material; the optimal group, i.e., water−cement ratio of 0.5, fly ash of 5%, Na 2 SO 4 of 1%, Ca(OH) 2 of 0.75%, and PVA fibers of 0.8%, is obtained by the orthogonal test method, which is the closest to the actual needs of the project. The hydration products of the optimized materials have obvious changes, and the needle-like AFt and C−S−H increase so that the performance of the materials has been significantly improved.