Use ColorAnimationUsingKeyFrames to animate GradientStop
<UserControl x:Class='SilverlightApplication3.MainPage'
xmlns='http://schemas.microsoft.com/winfx/2006/xaml/presentation'
xmlns:x='http://schemas.microsoft.com/winfx/2006/xaml'
xmlns:d='http://schemas.microsoft.com/expression/blend/2008'
xmlns:mc='http://schemas.openxmlformats.org/markup-compatibility/2006'
mc:Ignorable='d'
d:DesignWidth='640'
d:DesignHeight='480'>
<StackPanel Margin="15">
<TextBlock Name="label" TextAlignment="Center" Foreground="Blue" />
<Rectangle Name="rect" Width="200" Height="100" Stroke="Blue" Margin="10">
<Rectangle.Fill>
<LinearGradientBrush StartPoint="0,0" EndPoint="1,0">
<GradientStop Offset="0" />
<GradientStop Offset="1" />
</LinearGradientBrush>
</Rectangle.Fill>
</Rectangle>
<StackPanel.Triggers>
<EventTrigger RoutedEvent="StackPanel.Loaded">
<EventTrigger.Actions>
<BeginStoryboard>
<Storyboard>
<ColorAnimationUsingKeyFrames
Storyboard.TargetName="rect"
Storyboard.TargetProperty="Fill.GradientStops[0].Color"
RepeatBehavior="Forever">
<LinearColorKeyFrame Value="#FF00FF" KeyTime="0:0:0" />
<LinearColorKeyFrame Value="#00805A" KeyTime="0:0:5" />
<LinearColorKeyFrame Value="#FF0000" KeyTime="0:0:10" />
<LinearColorKeyFrame Value="#0000FF" KeyTime="0:0:15" />
<LinearColorKeyFrame Value="#00FFFF" KeyTime="0:0:20" />
<LinearColorKeyFrame Value="#FF00FF" KeyTime="0:0:25" />
</ColorAnimationUsingKeyFrames>
</Storyboard>
</BeginStoryboard>
</EventTrigger.Actions>
</EventTrigger>
</StackPanel.Triggers>
</StackPanel>
</UserControl>
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