ZnO nanoparticles were successfully synthesized using a microwave method, whose surface was modified with {4‐[(E)‐2‐(furan‐2‐yl)ethenyl]pyridin‐1‐ium‐1‐yl}acetate as a capping agent (1 and 3%). Their structural properties were investigated using FTIR, XRD, SEM, EDS, and UV–visible spectroscopy. XRD confirmed the Wurtzite structure for all compounds, a size of 30.6 nm for uncapped and 22.9 nm for 3% dye‐capped nanoparticles were calculated from Scherer's equation. Hexagonal wurtzite shape of nanoparticles can be clearly seen in the SEM images. The DFT calculations were carried out using quantum espresso. These dye‐capped ZnO nanoparticles were proved to be potential antibacterial agents, the minimum concentrations of dye‐capped ZnO nanoparticles that inhibit the growth of bacteria are 1.5 mg/mL for Escherichia coli and 0.78 mg/mL for Bacillus subtilis, which are much lower than those of uncapped ZnO. The bioactivity data suggest these organic–inorganic hybrid nanoparticles emerged as a new class of antibacterial agents.