Natural zeolites are used as adsorbents in purification processes due to their cation-exchange ability and molecular sieve properties. Surface modified natural zeolites (SMNZs), produced by attaching cationic organic surfactants to the external surface, can simultaneously act as ionic exchangers and organic molecule adsorbents. In this paper, SMNZs were produced and investigated as adsorbents for As(V) removal from wastewater: two natural zeolites, clinoptilolite and phillipsite, were modified using HDTMA-Br and HDTMA-Cl as surfactants. The obtained samples were then characterized under static and dynamic conditions. Results showed that As(V) removal follows a pseudo-second order kinetic, with fast adsorption rates: every sample reached 100 % removal in 2 h, while equilibrium data showed a Langmuir-like behavior, with a greater anion uptake by the HDTMA-Br modified SMNZs due to the formation of a compact and complete micellar structure. Finally, fixed-bed tests were performed to characterize the samples under dynamic conditions assessing the effect of severe operating parameters on the dynamic exchange capacity, selectivity and efficiency of the process. The obtained results demonstrate a good ability of the tested materials to adsorb As(V) from wastewater, confirming the effectiveness of the proposed surface modification technique in expanding the possibility of using natural zeolites in these processes.