Abstract: A silicon-containing isocyanate compound represented by the following general formula [I]: ##STR1## wherein each of R.sup.1, R.sup.2, and R.sup.3 independently represents a hydrocarbon group having 1 to 10 carbon atoms, an alkoxy group having 1 to 6 carbon atoms or a trialkyl siloxy group (each alkyl having 1 to 4 carbon atoms), with the proviso that at least one of R.sup.1, R.sup.2, and R.sup.3 is an alkoxy group having 1 to 6 carbon atoms, and n is a number of from 1 to 4, can be obtained in a high yield by reacting carbonyl chloride with a silicon-containing alkylamine represented by the following general formula [II]: ##STR2## wherein R.sup.1, R.sup.2, R.sup.3, and n are as defined above, in an inert organic solvent in the presence of a tertiary amine.