Two novel lanthanide metal–organic framework (Ln‐MOF) luminescent sensors for the detection of picric acid have been successfully assembled. Following a function‐oriented strategy, urea hydrogen‐bonding functional sites were introduced into two MOF frameworks. A structural analysis indicated that the two MOFs have the exact same structure, namely 2D layers with diamond‐shaped holes that are accumulated into a 3D framework through the hydrogen‐bonding interactions between urea and carboxylate groups. Interestingly, only half of the urea units are involved in supporting the MOF framework through N−H⋅⋅⋅O hydrogen‐bonding interactions, whereas the other half are located in the pore channel and act as empty recognition sites. Abundant N−H urea bonds are present in the inner walls of three types of interpenetrating 1D channels. Luminescence studies revealed that the two Ln‐MOFs exhibit high sensitivity, good selectivity, and a fast luminescence quenching response towards picric acid. In particular, the two Ln‐MOFs can be simply and quickly regenerated, and exhibit excellent recyclability. In summary, we have successfully used a function‐oriented strategy to achieve multiple functions in a ligand to construct lanthanide MOF luminescent sensors for the detection of picric acid, thereby providing a potential strategy for the future development of MOF luminescent sensors with a specific target.