Super-hard nanocomposite coatings have been received a great attention during recent years. Based on our previous investigations onto the several super-hard nanocomposite coating systems including nc-TiN/a-Si3N4,nc-TiN/a-BN. This paper reports on the nc-(Ti1-xAlxN)/a-Si3N4 nanocomposite coatings prepared by direct current plasma enhanced chemical vapor deposition (PECVD). And the effect of aluminum contents on the microstructure and hardness of the coatings have been mainly investigated. The coatings were characterized by means of X-ray diffraction (XRD),X-ray photoelectron spectroscopy (XPS), scanning electron microscopy (SEM) equipped with energy dispersive analysis of X-rays (EDX), and the hardness measurements were done by means of the automated load-depth sensing technique using Vickers diamond indenter. The thermal stability of nanocomposite coatings of TiN/a-Si3N4 was evaluated by annealing at elevated temperatures up to 1000℃. The results shows that super hardness of nc-(Ti1-xAlxN)/a-Si3N4 could be obtained with a wide aluminum content from 10at.% to 86at.% in (Ti1-xAlx)N phase, while the silicon content can be kept at 4～5 at.%. These nanocomposite coatings shows a relatively better thermal stability of nanocrystallite size and therefore high hardness up to 1000℃, which further support our earlier concept for the design of super-hard nanocomposite coatings. These results are suggested mainly due to the formation of nanostructure, and this indicates that the aluminum has also the role of controlling the crystallite size within nc-(Ti1-xAlxN)/a-Si3N4 besides its known well property of the super anti-oxidation.