This paper focuses on an in situ interfacial polymerization modification of polyamide thin film composite membranes with acrylic acid (AA) and zinc oxide (ZnO) nanoparticles. Consequent to this modification, the modified polyamide thin film composite (PA–TFC) membranes exhibited enhanced water permeability and Pb (II) heavy metal rejection. For example, the 0.50:1.50% ZnO/AA modified membranes showed water permeability of 29.85 ± 0.06 L·m−2·h−1·kPa−1 (pH 3), 4.16 ± 0.39 L·m−2·h−1·kPa−1 (pH 7), and 2.80 ± 0.21 L·m−2·h−1·kPa−1 1 (pH 11). This demonstrated enhanced pH responsive properties, and improved water permeability properties against unmodified membranes (2.29 ± 0.59 L·m−2·h−1·kPa−1, 1.79 ± 0.27 L·m−2·h−1·kPa−1, and 0.90 ± 0.21 L·m−2·h−1·kPa−1, respectively). Furthermore, the rejection of Pb (II) ions by the modified PA–TFC membranes was found to be 16.11 ± 0.12% (pH 3), 30.58 ± 0.33% (pH 7), and 96.67 ± 0.09% (pH 11). Additionally, the membranes modified with AA and ZnO/AA demonstrated a significant pH responsiveness compared to membranes modified with only ZnO nanoparticles and unmodified membranes. As such, this demonstrated the swelling behavior due to the inherent “gate effect” of the modified membranes. This was illustrated by the rejection and water permeation behavior, hydrophilic properties, and ion exchange capacity of the modified membranes. The pH responsiveness for the modified membranes was due to the –COOH and –OH functional groups introduced by the AA hydrogel and ZnO nanoparticles.