ItemsControl无法选择项目，只能显示集合。只有Selector或它的一个子代可以选择项目。
对于您的场景，我认为ListView和GridView是合适的。当用户单击行中的控件时，事件将冒泡到ListView，并且该项将被选中。您可以覆盖默认样式，这样它就不会显示为选中的行：WPF ListView turn off selection。

您可以使用ListView，并添加一个SelectionChanged事件，然后实现一个函数来验证ListView.SelectedItem，就像验证DataGrid一样

我有一个解决方案给你...一个行为：

public static class SelectedItemBehavior
   {
      public static readonly DependencyProperty BindingProperty =
         DependencyProperty.RegisterAttached("Binding", typeof(object), typeof(SelectedItemBehavior),
            new FrameworkPropertyMetadata(new object(),
               FrameworkPropertyMetadataOptions.BindsTwoWayByDefault,
               SelectedItem_Changed));

      public static object GetBinding(FrameworkElement frameworkElement)
      {
         return (object)frameworkElement.GetValue(BindingProperty);
      }

      public static void SetBinding(FrameworkElement frameworkElement, object value)
      {
         frameworkElement.SetValue(BindingProperty, value);
      }

      private static void SelectedItem_Changed(Object sender, DependencyPropertyChangedEventArgs e)
      {
         ToggleButton toggleButton = (ToggleButton)sender;
         toggleButton.Checked -= ToggleButtonOnChecked;
         toggleButton.IsChecked = e.NewValue?.Equals(toggleButton.DataContext) ?? false;
         toggleButton.Checked += ToggleButtonOnChecked;
      }

      private static void ToggleButtonOnChecked(object sender, RoutedEventArgs e)
      {
         ToggleButton toggleButton = (ToggleButton)sender;
         SetBinding(toggleButton, toggleButton.DataContext);
      }
   }

然后按如下方式进行绑定：

<ItemsControl
        Name="ItemsControlList"
        Width="200"
        Height="100"
        ItemsSource="{Binding Values}">
        <ItemsControl.ItemTemplate>
            <DataTemplate>
                <RadioButton local:SelectedItemBehavior.Binding="{Binding ElementName=ItemsControlList, Path=DataContext.SelectedValue}" Content="{Binding}" />
            </DataTemplate>
        </ItemsControl.ItemTemplate>
    </ItemsControl>