Water pollution is one of the most pervasive problems afflicting people all over the world, while adsorption is the most impactful method to remove the organic pollutants from water. To demonstrate this, a facile and efficient approach is extendable to prepare porous polyurea monolith as a new type of adsorbent for water purification in our research. In order to obtain the porous polyurea monolith, the reaction only between TDI monomer and vapor by using the centrifugally spinning moulding is prepared. Notably, the results show that centrifugally spinning moulding is an effective method to form the whole block structure. According to the specific surface area, pore size and pore size distribution of porous polyurea monolith are affected at different centrifugal speeds. The porous polyurea monolith has continuous interconnected fiber-like clusters skeletal structure, which is composed of mesopores and maropores. Moreover, the porous polyurea monolith could adsorb oils and organic solvents from water fast, which can be attribute to its highly hydrophobic and oleophilic properties.