The antibacterial tetracationic tetra-p-guanidinoethylcalix[4]arene developed by our team has been anchored through bottom-up or top-down pathways to the surface of Merrifield and Wang benzaldehyde resins; the attachment involved either a pyridinium linker or an imine/amine one. The grafting yields were evaluated by elemental analysis through the nitrogen content. Their sequestering properties towards bacteria were evaluated, using E. coli as a model, by capillary electrophoresis (CE) which showed their efficiencies and their bacteriophilic behaviors. All the new materials were compared to two pyridinium-derived Merrifield resins in terms of effective capture, efficiency, and removal coefficients, showing that some of these calixarene-derived resins are good bacteriophilic materials. Confirmation of such behavior has been provided by microscopy.