Expanding the specific surface area of substrates and carrying out precise surface engineering of imprinted nanocavities are crucial methods for enhancing the identification efficiency of molecularly imprinted polymers (MIPs). To implement this synergistic strategy, bioinspired surface engineering was used to incorporate dual covalent receptors via precise post-imprinting modifications (PIMs) onto mesoporous silica nanosheets. The prepared sorbents (denoted as “D-PMIPs”) were utilized to improve the specific identification of adenosine 5′-monophosphate (AMP). Significantly, the mesoporous silica nanosheets possess a high surface area of approximately 498.73 m²∙g^–1, which facilitates the formation of abundant specific recognition sites in the D-PMIPs. The dual covalent receptors are valuable for establishing the spatial orientation and arrangement of AMP through multiple cooperative interactions. PIMs enable precise site-specific functionalization within the imprinted cavities, leading to the tailor-made formation of complementary binding sites. The maximum number of high-affinity binding sites (N_max) of the D-PMIPs is 39.99 μmol∙g^–1, which is significantly higher than that of imprinted sorbents with a single receptor (i.e., S-BMIPs or S-PMIPs). The kinetic data of the D-PMIPs can be effectively described by a pseudo-second-order model, indicating that the main binding mechanism involves synergistic chemisorption from boronate affinity and the pyrimidine base. This study suggests that using dual covalent receptors and PIMs is a reliable approach for creating imprinted sorbents with high selectivity, allowing for the controlled engineering of imprinted sites.