The adoption of new synthesis strategy and monomers significantly promotes the construction of porous organic polymers (POPs) and their promising applications. A fabricating method of porous polyimides is developed via sequential imidization and cross‐linking reaction among self‐condensable building blocks, as reported in the authors' previous manuscript. Herein, porous polyureas (A‐POPs) are prepared starting from 4‐ethynylaniline and diisocyanate monomers, while porous polyamides (B‐POPs) are synthesized from 4‐ethynylbenzoic acid and diisocyanate monomers. It is found that decreasing the monomer content in solvent can effectively inhibit the premature phase separation and facilitate the evolution of integrated network. Eventually, a maximum surface area of 425 m2 g−1 is achieved for porous polyureas when the content of monomers is 10%. To the best knowledge, A‐POPs are the porous polyureas with the highest surface areas reported up to now. The as‐prepared porous polyurea (AN‐POP) exhibits the maximum adsorption capacity of 1093.87 ± 5.23 mg g−1 and removal rate of 99.96% for Au(III), due to its high surface area and the coordination between the heteroatoms (N and O) in A‐POPs and metal ions. Besides, the porous polyurea also exhibits excellent renewable efficiency and high selectivity to Au(III).