In this research Manganese-substitution impact on linear and nonlinear (NL) optical properties of Aluminum-doped ZnO (AlZnO) Nanoparticles (NPs) are investigated. Utilizing measured data of reflectance acquired from the DRS, the higher-order NL optical characteristics of the provided NPs are examined. The maximum quantity of NL susceptibility χ^3 is measured to be around 3.945×10-10 esu at wavelength λ=520 nm and 7.467×10-11 esu at wavelength λ=530 nm for AlZnO and Manganese-substituted Aluminum-doped Zinc-Oxide (Mn-also) NPs, for particle sizes 14−67 nm and 11−54 nm, consecutively. Consequently, the synthesis method (sol-gel) which is used in this work concluded a decrease in particle size and different optical behavior especially in UV spectral regions during the substitution with Manganese in comparison with the AlZnO. This decrement assures that a decrease in the size of crystallite induces a decline in the χ^3. The obtained optical parameters are red shifted with the Manganese substitution. Also, the NL absorption coefficient (βc(m/W)) is enhanced in the UV range. The maximum of the NL absorption coefficient (βc(m/W)), for AlZnO and Mn-AlZnO NPs, are determined (at λ =250 nm) 2.24×10-18 (m/W) and 5.76×10-15 (m/W) respectively.