The wettability of alumina toughened zirconia (ZTA) by Al-Mg alloy was investigated using the sessile drop technique. The effects of nickel coating, magnesium content, nitrogen atmosphere, and processing temperature on the contact angle between the molten alloy and the substrate were determined. Likewise, the effect of these factors on the wetting properties was studied. The results showed that the nickel coating on the ceramic substrate caused a significant reduction in solid/liquid surface energy and the contact angle decreased obviously. The presence of magnesium in the molten aluminum alloy in nitrogen atmosphere reduced the contact angle effectively. The presence of magnesium in the alloy must be at a minimum amount of 2wt%–3wt%. Moreover, it was suggested that some chemical reactions in the Al-Mg-N system led to the production of Mg3N2 and AlN compositions. These compositions improved the wetting properties of the systems by reducing the surface energy of the molten. It was shown that increasing the temperature is also an effective factor for the enhancement of wetting properties.