N-Halamine-based antibacterial materials play a significant role in controlling microbial contamination, but their practical applications are limited because of their complicated synthetic process and indistinct antibacterial actions. In this study, novel antibacterial N-halamine-containing polymer fibers were synthesized via an one-step electrospinning of N-halamine-containing polymers without any additives. By adjusting the concentration of precursor and the molecular weight of polymers, the morphology and size of the as-spun N-halamine-containing fibers can be regulated. The as-spun fibers showed antibacterial activity against both Gram-positive and Gram-negative bacteria. After an antibacterial assessment using different biochemical techniques, a combined mechanism of contact/release co-determined killing action was evidenced for the as-spun N-halamine-containing fibers. With the aid of contact action and/or release action, this combined mechanism can allow N-halamines to attack bacteria, making the as spun fibers wide in the application of antibacterial fields, whatever it is in dry or wet environment. Also, a recycle antibacterial test demonstrated that the as-spun fibers can still offer antibacterial property after five recycle experiments.