You can use the Chart.CustomizeLegend event to customize the alignment and separators for the legend items:
Imports System.Drawing
Protected Sub Chart_CustomizeLegend(sender As Object, e As CustomizeLegendEventArgs)
For Each item As LegendItem In e.LegendItems
' Align the series symbol.
item.Cells(0).Alignment = ContentAlignment.TopCenter
' Add a separator.
item.SeparatorType = LegendSeparatorStyle.Line
item.SeparatorColor = Color.LightGray
Next
End Sub
Protected Sub Page_Load(sender As Object, e As EventArgs) Handles Me.Load
Dim chart1 As New Chart
' Bind to the CustomizeLegend event.
AddHandler chart1.CustomizeLegend, AddressOf Chart_CustomizeLegend
Page.Controls.Add(chart1)
chart1.ChartAreas.Add(New ChartArea)
Dim l As New Legend
' ... The rest of your code...
End Sub