Databinding of RadioButtonList using SelectedValue...possible?

I am databinding a GridView to an object datasource. The gridview contains a TemplateField which contains a RadioButtonList with ListItems defined inline.
I want to be able to databind the SelectedValue of the RadioButtonList to the same underlying table as the other grid columns, but it doesn't work!

Do I have my syntax wrong, or is this impossible and requires looping code to individually select the proper item in each row?

<llblgenpro:LLBLGenProDataSource ID="llbComputerApplication" DataContainerType="EntityCollection" runat="server"></llblgenpro:LLBLGenProDataSource>
        <asp:GridView ID="gridComputerApps" DataSourceID="llbComputerApplication" runat="server" AutoGenerateColumns="False" 
            EmptyDataText ="NO APPLICATIONS FOUND FOR THIS COMPUTER." 
            DataKeyNames="ComputerID, ApplicationID" EnableViewState="False"
            style="border-style:dotted;border-width:thin"
            >
            <Columns>
                <asp:BoundField DataField="ApplicationID" HeaderText="Application ID" SortExpression="ApplicationID" Visible="True" />
                <asp:TemplateField HeaderText="Application Name"><ItemTemplate><%#Eval("Application.ApplicationName")%></ItemTemplate></asp:TemplateField>
                <asp:TemplateField HeaderText="Normalized Name"><ItemTemplate><%#Eval("Application.NormalizedAppName")%></ItemTemplate></asp:TemplateField>
                <asp:TemplateField HeaderText="Notes"><ItemTemplate><%#Eval("Application.NormalizedNotes")%></ItemTemplate></asp:TemplateField>
                <asp:TemplateField>
                    <HeaderTemplate>
                    </HeaderTemplate>
                    <ItemTemplate>
                        <asp:RadioButtonList SelectedValue='<%#Eval("RequirementOption")%>' ID="rblRequirementOption" RepeatDirecti