We demonstrate the synergistic effects of combining atmospheric pressure plasma generation together with aerosolization of the resultant plasma‐activated water using direct current electrospraying for effective chemical‐free spray‐based surface disinfection. Besides facilitating the efficient aerosol generation of the atmospheric pressure plasma pretreated water, the DC electrospray itself also constitutes a secondary plasma generation source that can further enhance the plasma‐activation of water to result in a further increase in the concentration of reactive species in the aerosols. This, in turn, can be seen to translate into an enhancement in bacteria inactivation efficacy. Additionally, we show that pretreating stainless steel surfaces using this hybrid spray‐deposition technique before pathogen exposure leads to almost complete inactivation of the bacteria colonies.