You need to use LinearLayout subviews. Like the user Price says:
There are limitations when using the GridLayout, the following quote is taken from the documentation.
"GridLayout does not provide support for the principle of weight, as
defined in weight. In general, it is not therefore possible to
configure a GridLayout to distribute excess space in non-trivial
proportions between multiple rows or columns ... For complete control
over excess space distribution in a row or column; use a LinearLayout
subview to hold the components in the associated cell group."
Here is a small example that uses LinearLayout subviews. (I used Space Views that takes up unused area and pushes the buttons into desired position.)
<GridLayout
xmlns:android="http://schemas.android.com/apk/res/android"
android:layout_width="match_parent"
android:layout_height="wrap_content"
android:columnCount="1"
>
<TextView
android:text="2x2 button grid"
android:textSize="32dip"
android:layout_gravity="center_horizontal" />
<LinearLayout
android:layout_width="match_parent"
android:layout_height="wrap_content"
android:orientation="horizontal">
<Space
android:layout_width="wrap_content"
android:layout_height="match_parent"
android:layout_weight="1" />
<Button
android:layout_width="wrap_content"
android:layout_height="wrap_content"
android:text="Button 1" />
<Space
android:layout_width="wrap_content"
android:layout_height="match_parent"
android:layout_weight="1" />
<Button
android:layout_width="wrap_content"
android:layout_height="wrap_content"
android:layout_gravity="start"
android:text="Button 2" />
<Space
android:layout_width="wrap_content"
android:layout_height="match_parent"
android:layout_weight="1" />
</LinearLayout>
<LinearLayout
android:layout_width="match_parent"
android:layout_height="wrap_content"
android:orientation="horizontal"
>
<Space
android:layout_width="wrap_content"
android:layout_height="match_parent"
android:layout_weight="1" />
<Button
android:layout_width="wrap_content"
android:layout_height="wrap_content"
android:text="Button 3" />
<Space
android:layout_width="wrap_content"
android:layout_height="match_parent"
android:layout_weight="1" />
<Button
android:layout_width="wrap_content"
android:layout_height="wrap_content"
android:layout_gravity="start"
android:text="Button 4" />
<Space
android:layout_width="wrap_content"
android:layout_height="match_parent"
android:layout_weight="1" />
</LinearLayout>
</GridLayout>
Check Price's response for more information.