The localized surface plasmon dynamics of laser ablated gold and gold-silver alloy nanoparticles (NPs) near interband and intraband excitation wavelengths were investigated using femtosecond (fs) transient absorption spectroscopy. Interband excitation with 70 fs laser pulses at a wavelength of 400 nm demonstrated plasmon photo-bleach and a transient absorption in the wings of the bleach spectrum. With intraband excitation, Ag50Au50 alloy NPs depicted a fast electron thermalization time of ~180 fs. A slower decay of positive absorption from alloy NPs was observed when compared to pure Au NPs. These NPs demonstrated a rapid initial electron thermalization and exhibited similar electron-phonon relaxation times. The third-order nonlinear optical (NLO) properties were measured using the Z-scan technique with 1 kHz repetition rate fs pulses at 800 nm. It is observed that the alloy NPs possessed large value of the NLO susceptibility χ(3) (~10−13 esu) compared to pure gold NPs at 800 nm finding applications in different areas of photonics. © 2019 Elsevier B.V.