Diamagnetic susceptibilities of 21 organic derivatives of silicon containing Si-O bonds are reported. χsi in these compounds has been calculated either graphically or from Pascal's additivity rule, and the reasons for the variation of χsi have been discussed, χm of these silicon compounds has also been calculated theoretically from different wave-mechanical approaches.1,2 A poor agreement has been obtained between the observed xm values and the corresponding values calculated according to Baudet and coworker's method, and this poor agreement has been analyzed in the light of different environmental conditions present in these molecules. An excellent agreement is obtained between experimental and calculated values from Hameka's method, χm values have been discussed and attributed to due considerations for the structural factors present in these silicon molecules which do contribute toward the molecular diamagnetism. © 1969, American Chemical Society. All rights reserved.