To develop efficient heterogeneous catalytic systems for base‐catalyzed reactions, two benzimidazole‐containing porous organic polymers, BPOP‐1 and BPOP‐2, were synthesized. As a result of the difference in building units, BPOP‐1 exhibits a granular morphology, and BPOP‐2 is composed of tiny particles. N2 adsorption measurements show that BPOP‐1 is a nonporous framework, whereas BPOP‐2 displays good adsorption abilities towards N2, H2, and CO2. Both BPOP‐1 and BPOP‐2 exhibit a higher catalytic activity in the Knoevenagel condensation reaction than their homogeneous molecular counterpart, and the activity of BPOP‐2 is superior to that of BPOP‐1. Theoretical calculations show that the Lewis basicity of the N atoms in BPOP‐1 is identical to that in BPOP‐2. The prominent catalytic performance of BPOP‐2 is mainly attributed to its high specific surface area and microporous character. Moreover, the permanent chemical stability of the structural framework endows BPOP‐2 with an outstanding recyclability.