UnRegisterTypeLib

[DllImport("oleaut32.dll", CharSet = CharSet.Unicode, PreserveSig = false)]
public static extern void UnRegisterTypeLib(
   [MarshalAs(UnmanagedType.LPStruct)] Guid libID,
   short wVerMajor,
   short wVerMinor,
   int lcid,
   SYSKIND syskind
);

Microsoft documentation: Link