In this study, we synthesized two novel metal–organic frameworks [Cd(C4H4N2)(C12H19P3O9)]n (1) and {Ca[Cd(H2O)3]2(C24H15N6O6)2}n (2) distinguished by exceptional fluorescence properties. Focusing on 1, we innovatively combined it with hydroxypropyl cellulose (HPC) to create a pH-responsive, fluorescence-guided nanocarrier system (HPC-1@DOX) for targeted delivery of doxorubicin (DOX) in cancer treatment. We thoroughly evaluated the loading and release efficiency of DOX under varied pH conditions, demonstrating sustained and controlled drug release characteristics in vitro, along with substantial drug-loading capacity. Notably, HPC-1@DOX exhibited pH-responsive behavior, releasing DOX preferentially at pH 6.8, indicative of targeted delivery to tumor and inflammatory sites while minimizing release at higher pH values. Moreover, we explored its biological impact, confirming HPC-1@DOX’s ability to up-regulate miR-493-3p expression in lung carcinoma cells, thereby inhibiting proliferation, reducing invasiveness, and inducing apoptosis. This multifunctional nanocarrier system represents a significant advancement towards targeted and effective cancer therapy.