Catalytic cracking of n-decane was performed over monometallic and bimetallic Pt-Ni catalyst supported La-Al2O3 modified by MoO3 (MLA), aiming to investigate the effects of acidity, active phase dispersion, and synergistic effect between Pt and Ni on catalytic performance of the catalysts. The catalysts were characterized by the techniques of Brunauer-Emmett-Teller (BET), hydrogen temperature-programmed reduction (H-2-TPR), X-ray diffraction (XRD), temperature-programmed desorption of ammonia (NH3-TPD), X-ray photoelectron spectroscopy (XPS), CO chemisorption, and transmission electron microscopy/energy-dispersive spectroscopy (TEM/EDS) mapping. The results showed that catalytic cracking activities over catalysts were heightened compared with MLA, especially bimetallic catalyst. Meanwhile, bimetallic catalyst exhibited the best high-temperature stability. Otherwise, cracking activity over regenerative bimetallic catalyst nearly approached that of the fresh one. The most effective findings of properties of bimetallic catalyst presented as follows: the unique acidity, higher resistance against sintering of active phases, and finely dispersed actives due to enhanced metal-support interaction and synergistic effect between Pt and Ni can be responsible for its stable catalytic activity and thermal stability, and capable regeneration.