Zwitterions are neutrally charged molecules with an equal number of cationic and anionic groups. Their exceptional fouling resistance makes them excellent membrane materials. This study focuses on thin-film composite (TFC) ultrafiltration membranes where the selective layers consist of zwitterion-containing hydrogels. To synthesize these membranes with ultra-thin hydrogel selective layers we used a novel method, Interfacially Initiated Free Radical Polymerization (IIFRP). While previous studies focused on poly(ethylene glycol) (PEG)-based selective layers, we aimed to determine the effect of incorporating two zwitterionic monomers, sulfobetaine methacrylate (SBMA) and 2-methacryloyloxyethyl phosphorylcholine (MPC), on permeability, selectivity, and fouling resistance. Compared to a PEG-based hydrogel selective layer, all zwitterion-containing hydrogel selective layers showed increased water permeance (12.2 ± 1.8 L/m2 h bar for SBMA, 7.3 ± 1.8 L/m2 h bar for MPC). Interestingly, this permeance increase was not accompanied by a major decrease in protein rejection despite the zwitterion-containing hydrogels having lower chemical cross-link densities, with myoglobin rejections staying >90%. This was likely due to physical cross-links between zwitterionic moieties. For the same total monomer concentration, higher zwitterion concentrations led to a permeance increase of almost an order of magnitude along with only minimal decrease in protein rejection. Moreover, all hydrogel selective layer TFC membranes tested exhibited excellent oil fouling resistance.