The growing demand of zeolites for many industrial applications has led to a search for eco-friendly alternatives for their production, in an attempt to reduce costs, save natural resources and alleviate the associated environmental impacts. In the present study, hazardous aluminum salt slag (aluminum source) and rice husk ash (silicon source) were used as secondary raw materials to synthesize sustainable NaP-type zeolites through a hydrothermal process. A central composite rotational experimental design was applied to evaluate the effect of the reaction time and hydrothermal temperature on the obtained zeolites crystallinity. Using the proposed experimental design, temperatures between 85 and 115 °C and different reaction times (2–28 h) were tested. It was found that the interaction between the variables (time and temperature) and both variables, independently, exerted a significant influence on the crystallinity of the zeolites. The optimal experimental conditions (105 °C and 20 h), statistically determined, enabled a high degree of crystallinity (>73%) to be achieved. Thus, the use of hazardous aluminum and agri-food wastes as unconventional precursors for the production of zeolites represents a sustainable alternative to manage these wastes, by transforming them into secondary raw materials.