Electroless nickel plating generates substantially more waste than other metal-finishing processes due to the inherent limited bath life and the need for regular bath disposal. Electrodialysis can be used to regenerate electroless nickel baths, but poor membrane permselectivity, leading to high losses of valuable bath components, continues to be a weakness of the technology, This research has investigated improving electrodialysis permselectivity for removing contaminants (sodium, orthophosphite, and sulfate) in a spent electroless nickel bath while minimizing the losses of valuable bath ions (nickel, hypophosphite, and organic acids). Ion permselectivity was explored with respect to electrodialysis operating conditions, membrane type, and cell configuration. Excellent permselectivity for sodium over nickel was attained irrespective of operating condition, membrane, or cell configuration. Studies on the effects of four different operating conditions (current density, pH, flow rate, and temperature) on anion permselectivity revealed bath pH and current density to be critical operating parameters. The type of anion exchange membrane used had a crucial effect on selectivity; one membrane (Ionac MA-3475) was identified as having superior selectivity for bath contaminants particularly for sulfate. The improvements in electrodialysis permselectivity established by this research will decrease waste generation within the electroless nickel process and increase resource productivity by minimizing the loss of valuable plating chemicals.