As John says, the first stage is to get 4 wheel alignment done to get a known baseline before modifying anything.
I have 195/50 & 205/50 tyres on a TC car but with adjustable suspension so perhaps my settings won't translate to your car. Even so, they are broadly in line with the OEM settings and I aim for mid-range on toe settings, low end on rear camber. The ride height is also slightly lower than OEM. Front camber isn't adjustable on my car so I hope it's standard !
The image shows the details recorded almost 4yrs ago and with a mixture of imperial & metric numbers but this was the last time I made any changes. I seem to recall moving the OSR toe closer to the NSR toe after this measurement going on the noted shims, but memory.....
When you say it's unstable at moderate speed, what's the effect ? is it vibration or the car responding violently to bumps, road camber, etc ? If it's definitely the front and your toe is within range then I'd look to see if there's anything wrong with the steering gear, maybe that coupling hidden in the chassis, the track rod ends, bearings, etc.
Brian