Although zeolite N (K12Al10Si10O40Cl2.8H2O) is used commercially for the removal and recovery of ammoniacal nitrogen from wastewater, it has received limited attention in academic literature. The hypothesis was that if an improved understanding of zeolite N synthesis and resultant physical parameters and performance can be acquired, then the application of this material may be accelerated. This study successfully addressed existing research challenges including: maximizing the cation exchange capacity (CEC); selection of preferred synthesis conditions; control of the size, shape, and dispersion of zeolite N crystals; and improvement of ion exchange properties. Zeolite N was hydrothermally synthesised from kaolin clay added to solutions of potassium hydroxide and potassium chloride in a “one pot” process. CEC values increased to 563 meq/100 g (c.f. 528 meq/100 g in previous literature). Reaction between 120 and 140 °C for 2–4 h under static conditions was preferred as higher temperatures (180 °C) produced kalsilite. The KOH molarity (1.2–4.3 M) controlled the average zeolite crystal size, dispersion, and crystal shape; with highest molarity values optimal. Whereas, added KCl acted as a template which promoted zeolite N formation. Removal of KCl resulted in creation of zeolite F (K13(OH)3Al10Si10O40.13H2O) which also belonged to the EDI structural type. Ammonium ion exchange from aqueous solution was improved when diffusion restrictions were eased; as evidenced by using smaller zeolite crystals which were highly dispersed and not agglomerated. Not only was a greater cation capacity recorded but also the time to reach equilibrium was increased.