Layer-by-layer coating technique has been shown their considerable advantages including fast and mild process, flexibility and easy to scale up comes to the surface functionalizations. One of the most pronounced functionalities is the antimicrobial approach. We are aiming at developing non-complicated methods for antibacterial properties on different substrates mainly cellulose-based materials using alternative cationic polyelectrolytes, as well as having a better understanding of their antibacterial mechanisms. We found an interesting correlation between the surface positive charge and antibacterial efficiency, and the attractive force generated from oppositely charged surfaces is the key to deactivate the bacteria on contact. The bactericidal effect is more profound when the charged surface with micro/nano structures, which can lead to the disruption of the bacterial cell membrane more efficiently and kill the bacteria.