The synthesis of variable composition Au x Ag (1−x) alloyed nanoparticles prepared by laser ablation in water is reported. The nanoalloys exhibited a single characteristic surface plasmon resonance peak, whose spectral position was lying between the surface plasmon resonance peaks of neat Ag and Au nanoparticles, at about 400 and 530 nm respectively, depending directly on the composition of the alloyed nanoparticles. The nonlinear optical response of the nanoalloys was studied in details under 532 nm (visible) 35 ps and 4 ns laser excitation and it was found to be significant and greatly influenced by the position of the plasmonic band relative to the laser excitation wavelength. In this respect, increase of the Au molar fraction resulted in shifting of the nanoalloy plasmon band toward the location of the plasmon band of neat Au nanoparticles, i.e., at about 530 nm, closer to the laser excitation wavelength, hence causing more efficient resonance enhancement of the nonlinear optical response. Moreover, the nanoalloys were found to exhibit strong saturable absorption behavior when excited by ps or ns pulses, in the latter case this behavior changing to reverse saturable absorption at high laser intensity. The origin, the magnitude and the sign of the observed optical nonlinearities of the alloyed nanoparticles are explained and discussed in terms of the hot-electron and the interband contributions taking place under laser excitation in such nanostructures. The possibility of controlling the magnitude and the sign of the nonlinear optical response of Au x Ag (1−x) nanoalloys through their composition provides an attractive and efficient way to tailor the optical nonlinearities of noble metal nanoalloys, making them very useful for various emerging photonic, biophotonic, and optoelectronic applications.