To balance the board, fill layer3 with copper.
Rf?
Fill layer 3 with your power plane, not ground. Would I be right to guess that layer 3 is power routing anyway?
General comments:
Are you doing via in pad? Be aware that this can make soldering your components tricky. Ideally you should make sure the via is plated over, otherwise it wicks solder away from the joint. Even with this, soldering is harder as the via sucks heat from the joint.
If you have a high speed signal, place a ceramic decoupler close to any place the signal jumps from layer 1 to 4. A signal propagating on layer 1 will induce a equal and opposite current in the plane on layer 2.
What people new to high speed struggle with is that the current in the plane follows the path of the signal. The current in the plane will flow directly beneath the signal, not take the shortest path, or spread out over the whole plane.
When your signal jumps layers and references a new plane , you need to stich the reference planes to provide a path for the return current.
In your case, with a signal in layer 1, the return current is on the plane in layer 2. When signal jumps to layer 4, then the return current flows in the plane on layer 3.
So you need to stitch the planes together.
If the planes are the same (e.g. both GND) then just stitch with a via. If they are different (e.g. GND layer 2, VCC layer 3) stitch with a decoupling cap.
The stitching structure needs to be close to the signal via to minimise the loop area (inductance) between signal current and return current paths.
Also ensure that there is plenty of decoupling between power and ground at any IC or connector.
In general it looks like you need a lot more decoupling.
HTH