Polymeric materials that have been extensively applied in medical devices, wearable electronics, and food packaging are readily contaminated by bothersome pathogenic bacteria. Bioinspired mechano-bactericidal surfaces can deliver lethal rupture for contacted bacterial cells through mechanical stress. However, the mechano-bactericidal activity based only on polymeric nanostructures is not satisfactory, especially for the Gram-positive strain which is generally more resistant to mechanical lysis. Here, we show that the mechanical bactericidal performance of polymeric nanopillars can be significantly enhanced by the combination of photothermal therapy. We fabricated the nanopillars through the combination of low-cost anodized aluminum oxide (AAO) template-assisted method with an environment-friendly Layer-by-Layer (LbL) assembly technique of tannic acid (TA) and iron ion (Fe). The fabricated hybrid nanopillar exhibited remarkable bactericidal performances (more than 99%) toward both Gram-negative Pseudomonas aeruginosa (P. aeruginosa) and stubborn Gram-positive Staphylococcus aureus (S. aureus) bacteria. Notably, this hybrid nanostructured surface displayed excellent biocompatibility for murine L929 fibroblast cells, indicating a selective biocidal activity between bacterial cells and mammalian cells. Thus, the concept and antibacterial system described here present a low-cost, scalable, and highly repeatable strategy for the construction of physical bactericidal nanopillars on polymeric films with high performance and biosafety, but without any risks of causing antibacterial resistance.