The nonlinear optical properties of nanocomposites consisting of non-spherical silver nanoparticles in glass matrix have been studied using the femtosecond Z-scan technique. The spheroidal nanoparticles were uniformly oriented along a common direction. By polarization sensitive studies, longitudinal and transverse plasmon resonances can be addressed separately. A sign reversal in optical nonlinearity from negative to positive is observed while switching the light interaction from near to non-resonant regime, which can be done by simply rotating the light polarization by 90°. Studying samples with different aspect ratio, we obtained the dispersion of third-order nonlinearity in the near-resonant regime, showing an enhancement of the nonlinear processes by more than two orders of magnitude due to the electric field enhancement at the surface plasmon resonance.