To customize the Header HorizontalAlignmenet of the GroupChrome element you should edit the default GroupChromeStyle
and more specifically the GroupChromeTemplate
. Search for ContentControl inside it where its Content is TemplateBound to Header property. You'll see that its default HorizontalAlignment property is preset to Center -- change it to Stretch.
You can see where to find a control's style in the Editing Control Templates help article.
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