在博客的帮助下自己解决了这个问题。
据我所知,您无法在内部进行附加属性绑定。
下面将立即解决此问题(itemcontainerStyle!):
<DataTemplate DataType="{x:Type TestApp:GridVM}">
<ItemsControl ItemsSource="{Binding Path=Children}">
<ItemsControl.ItemContainerStyle>
<Style>
<Setter Property="Grid.Row" Value="{Binding GridRow}" />
<Setter Property="Grid.Column" Value="{Binding GridColumn}" />
</Style>
</ItemsControl.ItemContainerStyle>
<ItemsControl.ItemsPanel>
<ItemsPanelTemplate>
<Grid ShowGridLines="True" Style="{Binding Path=Style}">
<Grid.RowDefinitions>
<RowDefinition Height=".5*" />
<RowDefinition Height=".5*" />
</Grid.RowDefinitions>
<Grid.ColumnDefinitions>
<ColumnDefinition Width=".5*" />
<ColumnDefinition Width=".5*" />
</Grid.ColumnDefinitions>
</Grid>
</ItemsPanelTemplate>
</ItemsControl.ItemsPanel>
</ItemsControl>
</DataTemplate>