In summary, this work establishes a new paradigm for the precision engineering of 2D mesoporous materials. The interface-confined anisotropic assembly strategy not only overcomes long-standing challenges in structural control but also provides a versatile platform for designing advanced functional materials. By decoupling and independently tuning critical structural parameters, this approach opens new avenues for optimizing performance in a wide range of applications, from catalysis and energy storage to smart diagnostics and next-generation therapeutic platforms.