The carrier performance of palygorskite (Pal) can be significantly affected by its structure, morphology, and activity, which was regulated by controlling the dissolution degree of the metal-oxygen octahedron of raw Pal (RPal) under the action of oxalic acid (OA) in this study. The RPal and OA-leached RPal (OPal) then served as supports for immobilizing silver nanoparticles (AgNPs) to form RPal/AgNPs and OPal/AgNPs antibacterial nanocomposites. The structural and morphological characterizations were used to confirm the dispersion uniformity of AgNPs on the RPal and OPal nanorods, and antibacterial experiments were conducted to evaluate the performance of as-prepared composites and also investigate their antibacterial mechanism. The results showed that OPal-48h (OA leaching for 48 h) loaded with AgNPs (OPal-48h/AgNPs) possesses the most excellent and broad-spectrum antibacterial properties, where its minimum inhibitory concentration values against E. coli, S. aureus, ESBL-E. coli, and MRSA reached 0.25, 0.125, 0.25, and 0.5 mg/mL, respectively, which are mainly attributed to the optimal balance between surface activity and structural stability of OPal-48h that maximally increased its dispersibility and active sites, therefore contributing to the in situ formation of monodisperse AgNPs on the nanorods of OPal-48h.