Values of second-order polarizabilities (beta(xxx)), the composite magnitude (beta(CT microg)) of molecular hypersusceptibilities and the second harmonic generation (SHG) of microcrystal were used to characterize and evaluate the second-order nonlinear optical performance of 10-hydrocarbylacridones. Using Nd:YAG as a laser source, the SHG values of these compounds in powder as compared with urea powder were obtained, compared with the calculated values of beta(CT microg) and beta(xxx) found by solvatochromic method. The results showed that the SHG values of compounds 1, 2, and 5 are larger than that of urea. Compound 5 has a highest beta(CT microg) value among the 12 compounds. Although the different electronegativities of hydrocarbyl (R) attached to nitrogen atom should have an effect on the extent of intralmolecular charge-transfer and further influence SHG, beta(CT microg) or beta(xxx) values, the relationships between electronegativity of R and SHG, beta(CT microg) or beta(xxx) could not be found. But it is found that the bigger the donating-electron ability of R, the longer the maximum absorption wavelength of 10-hydrocarbylacridone molecules.